Review Reports

Comment 1

Novelty and critical analysis

The manuscript is comprehensive but is largely descriptive. The review would benefit from a more critical discussion comparing different synthesis routes, magnetic performances, and existing challenges. The authors should clearly identify the advantages and limitations of each approach instead of only summarizing published results.

Answer 1

We thank the reviewer for this valuable and constructive comment. We agree that the original submission treated the synthesis routes as a sequence of independent mechanistic descriptions without a direct critical comparison. To address this, we have added a new introductory paragraph followed by a comparative summary table (Table 2) at the end of the Precision Synthesis Methodologies section. The paragraph explicitly frames the trade-offs governing method selection, while the table provides a side-by-side comparison of all top-down and bottom-up routes discussed, including atomic-scale homogeneity, energy/temperature requirements, typical morphological outcome, and key limitations, allowing readers to directly weigh the advantages and limitations of each approach rather than reading them as isolated summaries. The added text is highlighted in the revised manuscript. we have highlighted the table in yellow

Comment 2

Literature coverage

Although many references are included, the authors should ensure that the most recent publications (particularly from the last two to three years) are adequately represented. The review would be strengthened by discussing the latest advances in entropy engineering, computational modelling, machine learning approaches, and application-oriented studies.

Answer 2

We thank the reviewer for this comment. We have conducted a systematic audit of the reference list and confirm that publications from the last three years (2023-2026) already constitute roughly half of all citations, including several from the current year. Nonetheless, to ensure the most recent developments are explicitly represented across all four areas raised by the reviewer, we have added three new references published within the last several months: (i) He et al. (2026, J. Mater. Chem. A) on synergistic interface and entropy engineering in ferrite/nitride high-entropy composites for microwave absorption, incorporated into the EMI shielding application section (Section VII.1); (ii) Santos et al. (2026, J. Chem. Inf. Model.) on large-language-model-assisted machine learning for single-phase high-entropy oxide design, incorporated into the Data-Driven Discovery subsection (Section VIII.3); and (iii) a recent computational study on machine-learning interatomic potentials for high-entropy oxide synthesizability prediction, incorporated into Section VIII.1.D. In the course of this audit, we also identified and corrected a duplicate citation (the same publication had inadvertently been assigned two separate reference numbers), which has been consolidated in the revised reference list. We believe these additions, together with the existing 2023-2025 coverage, ensure the review reflects the current state of the field across entropy engineering, computational modelling, machine learning, and application-oriented research.

Comment 3

Structure–property relationships

Greater emphasis should be placed on explaining how cation distribution, configurational entropy, lattice distortion, and synthesis conditions influence the magnetic properties. The discussion should move beyond qualitative descriptions and provide deeper physical interpretation.

Answer 3

We thank the reviewer for this insightful comment. We would like to clarify that the original manuscript already provided a quantitative, mechanism-level treatment of how cation distribution and lattice distortion govern magnetic exchange (Sections 3.1-3.3 and 4.1), including the ionic-mismatch formalism (Eq. 5) and the bond-angle dependence of the superexchange integral. However, we agree that the manuscript did not explicitly connect these mechanisms to the synthesis conditions described earlier, nor did it distinguish the nominal, composition-defined configurational entropy from the degree of disorder actually achieved through a given processing route. We have addressed this by adding a new subsection, 4.5 "Bridging Synthesis Pathway and Magnetic Outcome", which explicitly links the mechanical, chelation-based, combustion, and hydrothermal synthesis routes discussed earlier to their expected effects on exchange-integral distribution, spin-glass freezing, exchange bias, saturation magnetization, and anisotropy, and clarifies the distinction between nominal and kinetically realized configurational entropy. The added text is highlighted in the revised manuscript. We have highlighted the added part in yellow.

Comment 4

Applications

The section on applications would benefit from a more quantitative comparison. Including tables summarizing representative materials, synthesis methods, magnetic parameters (Ms, Hc, Tc), and application performance would significantly improve the usefulness of the review.

Answer 4

To further substantiate the structure-property discussion, we have added Table 4, compiling representative experimental Ms, Hc, and Tc values reported for realized high-entropy compositions in the two structural families most developed to date: spinel (Jin et al., 2023) and M-type hexaferrite (Lu et al., 2025). We note, and now explicitly state in the revised Challenges & Future Outlook section, that no experimentally realized high-entropy Y-type or Z-type hexaferrite (incorporating five or more simultaneous cations at a single sublattice) with reported magnetic parameters could be identified in the literature, which we highlight as an open synthetic opportunity rather than omit silently. We have highlighted the table in yellow

Comment 5

Future perspectives

The conclusion should provide a stronger outlook by identifying the key scientific challenges that remain unresolved, such as phase stability, reproducibility, scalability, computational prediction, and commercial applications.

Answer 5

We thank the reviewer for this comment. We would like to note that the original submission already provided substantial depth on two of the five areas raised: computational prediction (Sections VIII.1 and VIII.3, covering DFT+U/hybrid-functional modeling and machine-learning-driven discovery) and phase stability (Section VIII.2, on distinguishing true entropy stabilization from kinetically trapped metastability). However, we agree that reproducibility and scalability were mentioned only in passing, and commercial applications were not addressed at all. We have added a new subsection, IX. Practical Barriers to Translation: Reproducibility, Scalability, and Commercial Viability," which explicitly discusses (i) the sensitivity of realized configurational entropy to synthesis conditions and its consequences for batch-to-batch reproducibility, building on the synthesis property discussion in Section 4.4; (ii) the engineering challenges of scaling synthesis from laboratory to industrial batch sizes; and (iii) the cost-competitiveness and regulatory barriers to commercial market entry, with particular reference to the biomedical applications discussed in the manuscript . The added text is highlighted in the revised manuscript .

Comment 1

Several sections contain lengthy paragraphs that could be shortened for improved readability.

Answer 1

We thank the reviewer for this observation. We would like to clarify that the length of these paragraphs reflects a deliberate structural choice rather than an oversight. As this is a comprehensive mechanistic review rather than a short communication, several sections, particularly those addressing synthesis mechanisms, superexchange pathway derivations, and entropy-stabilization thermodynamics, present a continuous chain of cause-and-effect reasoning. For example, tracing how a given ionic-radius mismatch propagates through lattice distortion, to bond-angle deviation, to modification of the exchange integral, and ultimately to the resulting magnetic behavior, requires an uninterrupted narrative thread. Fragmenting this argumentative chain into multiple shorter paragraphs risks obscuring the causal linkages that are central to the critical, mechanism-level treatment this review aims to provide, particularly for readers less familiar with this rapidly developing field.

Nevertheless, in response to the reviewer's concern, we have revisited the manuscript and improved readability through complementary means that do not compromise mechanistic completeness: (i) bolded topic-sentence lead-ins have been added at the start of the longest paragraphs to aid navigation and signal their scope at a glance; (ii) several methodological comparisons have been consolidated into the newly added summary tables ( see our responses to the related comments above), offloading descriptive density from the running text; and (iii) paragraph boundaries have been reviewed throughout to ensure each paragraph corresponds to a single, self-contained mechanistic unit rather than spanning multiple ideas. We hope the reviewer agrees that these targeted adjustments improve readability while preserving the depth of argumentation that this review's scope requires.

Comment 2

Some statements describing magnetic mechanisms should be supported by additional references.

Answer 2

We thank the reviewer for this observation. Upon review, we identified several mechanistic passages, particularly concerning the Mössbauer spectral deconvolution protocol, the exchange-bias interfacial pinning mechanism, and the magnetocaloric response, that presented well-established physical reasoning without an explicit supporting citation at the point of the specific claim. We have addressed this by explicitly citing the following studies, already present in our reference list, at the corresponding statements: Cieslak et al. for the Mössbauer-based cation-distribution deconvolution methodology; Ghosh et al. and Sharma et al. for the exchange-bias pinning mechanism in spinel systems; and Peng et al. and Verma et al. for the magnetocaloric broadening discussion. The relevant additions are highlighted at each corresponding location in the revised manuscript.

Comment 3

Figures should have more informative captions and clearly indicate whether they are original or reproduced from published work. Appropriate permissions should be confirmed where necessary.

Answer 3

We thank the reviewer for this comment. We confirm that all figures in this manuscript are original and were created by the authors specifically for this review; none are reproduced or adapted from previously published sources, and therefore no third-party permissions were required. We further agree that the captions of the crystal-structure figures (Figs. 2-5) were comparatively brief relative to the mechanistic figures elsewhere in the manuscript. We have expanded these captions to explicitly state the space group and representative composition depicted, the crystallographic data source used to construct each structure, the rendering software employed, and a legend clarifying the color-coding of cation sites and coordination polyhedra. The revised captions are highlighted in the updated manuscript. All the edited captions have been highlighted in yellow

Comment 4

Please carefully check the consistency of terminology throughout the manuscript (e.g., High-Entropy Ferrites, HEFs, High-Entropy Oxides, spinel ferrites).

Answer 4

We thank the reviewer for this comment. We have carried out a full terminological audit of the manuscript to ensure each abbreviation consistently and correctly matches the term it represents throughout. Specifically, "high-entropy ferrites (HEFs)" is now used consistently wherever the discussion pertains to the Fe-based magnetic materials that are the specific subject of this review, while "high-entropy oxides (HEOs)" is retained only where the broader, non-ferrite-specific compositional family is genuinely intended  such as the historical introduction of the first entropy-stabilized oxide, which contains no iron, and other general references to the wider high-entropy ceramics field that are not specific to ferrites. This context-dependent correction ensures the two terms are no longer used interchangeably or as though they were parallel categories, while preserving the scientific accuracy of statements that genuinely concern the broader oxide family rather than ferrites specifically. All revised instances are highlighted in the updated manuscript.

Comment 5

Mathematical symbols, crystallographic notation, oxidation states, and chemical formulae should be formatted consistently throughout the manuscript.

Answer 5

We thank the reviewer for this comment. We have carried out a systematic check of crystallographic notation, oxidation-state formatting, and chemical formulae throughout the manuscript. Crystallographic space-group notation (e.g., Fd-3m, Pbnm) and chemical formula subscripting were confirmed to be consistently formatted throughout. We identified and corrected one inconsistency in oxidation-state notation (Zn⁺², which did not match the magnitude-then-sign convention (e.g., Fe³⁺, Co²⁺) used consistently elsewhere in the manuscript) and have unified it accordingly. The correction is highlighted in the revised manuscript.

Comment 6

The reference list should be carefully checked for formatting consistency and completeness.

Answer 6

We thank the reviewer for this comment. We have carried out a full, systematic review of all references in the manuscript, checking each entry for completeness (authors, title, journal, volume, page numbers, and year) and for consistency of formatting throughout. Several inconsistencies and incomplete entries were identified and corrected accordingly, including missing bibliographic details, an inconsistency in the formatting of book/chapter entries, and a duplicate citation, which has now been consolidated. The reference list has been fully updated and is reflected in the revised manuscript.

Comment 7

A thorough proofreading is recommended to correct minor grammatical issues, improve sentence structure, and eliminate typographical errors.

Answer 7

We thank the reviewer for this comment. We have carried out a thorough proofreading of the entire manuscript, correcting minor grammatical issues, refining sentence structure for clarity, and eliminating typographical errors throughout. The revised manuscript reflects these language and copyediting improvements.

Comment 1

In this review, if a figure is not original or is sourced from elsewhere, the corresponding reference must be added after the figure caption.

Answer 1

We thank the reviewer for this comment. We confirm that all figures included in this manuscript (Figures 1–17) are original and were created by the authors specifically for this review; none are reproduced, adapted, or sourced from previously published material. As such, no external references are required after the figure captions.

Comment 2

Add the latest literature on high-entropy ferrites from January to August/ 2026.

Answer 2

We thank the reviewer for this comment. We note that Reviewer 1 raised a related concern regarding recent literature, in response to which we already incorporated several recent references spanning entropy engineering, computational modelling, and machine-learning approaches for high-entropy materials. To specifically address the January-August 2026 window highlighted here, we have additionally incorporated a further recent study: N. Sharma et al., "Ultra-soft ferrimagnetism in a high-entropy spinel oxide driven by site-selective cation disorder," Materials Horizons (2026), reporting an exceptionally low coercivity (1.8 Oe) in a high-entropy spinel oxide. Together with the additions made in response to Reviewer 1, we believe the manuscript now reflects the most current literature available at the time of this revision. The new citation is highlighted at its corresponding location in the revised manuscript.

Comment 3

References: - In the part of References, please check all References. The Reference style of References does not agree with that of Magnetochemistry. Thus, all the References should be carefully checked and changed to the Reference style that agrees with that of Magnetochemistry.

Answer 3

We thank the reviewer for this comment. We have reformatted the entire reference list using the official MDPI reference style, applied via the EndNote MDPI style file, to ensure full consistency with the formatting required by Magnetochemistry. All references have been carefully checked following this conversion. The updated reference list is reflected in the revised manuscript.

Comment 1

The very idea of writing such a review is good. The authors deserve credit for this. However, the authors have not fulfilled the task they set out to do. The topic is engaging and captivating. However, the topic is not fully explored in the article. The authors write that the main goal of the review is to provide a systematic and comprehensive assessment of the rapidly evolving landscape of high‑entropy ferrites (HEFs), bridging the gap between fundamental thermodynamic principles and practical magnetic applications. By synthesizing the latest advances in precision synthesis ranging from chemical processes at the atomic scale to advanced sintering methods, this work aims to elucidate how configurational entropy can be used to stabilize complex single‑phase spinel and hexaferrite structures. However, this goal has not been achieved.

The authors describe the thermodynamic characteristics of a solid. They meticulously and in detail describe the crystal structure of spinel ferrites, Hexaferrites of type M, type Y, and type Z, as well as the crystal structure of orthoferrites. They describe methods for producing ferrites and some of their applications. However, all this information is available in textbooks, monographs, and review articles.

The manuscript does not present the relationships between quantitative thermodynamic characteristics, in particular entropy, and composition, properties, and technological characteristics.

In their work, the authors say nothing about garnet ferrites. These ferrites should primarily be classified as so‑called high‑entropy ferrites, since crystals with a garnet structure have a huge isomorphic capacity. Almost the entire periodic table can be introduced into the crystal lattice of a garnet ferrite.

The title of the article does not reflect its content. The manuscript contains no scientific novelty. In this regard, in my opinion, the manuscript should not be published in the journal “Magnetochemistry”.

Answer 1

We fully agree with the reviewer that the garnet lattice (A₃B₅O₁₂), with its three distinct dodecahedral, octahedral, and tetrahedral sublattices, possesses an exceptional isomorphic capacity that makes it, in principle, an outstanding candidate host for high-entropy design a point we explicitly acknowledge in our Introduction. However, our decision to concentrate the manuscript's in-depth structural, synthetic, and property analysis on the spinel and hexaferrite families reflects the current experimental maturity of the field rather than an oversight: to date, only a small number of single-phase high-entropy garnet ferrites have been successfully realized in the literature, in contrast to the substantially larger and more mature body of work available for spinel and hexaferrite systems, which alone comprises dozens of the studies synthesized in this review. Providing the same depth of critical, structure-property-level treatment for garnets that we provide for spinel and hexaferrite systems would, at this stage, require extrapolating well beyond what the primary literature currently supports. We have therefore chosen to flag high-entropy garnet ferrites explicitly as a promising and rapidly emerging direction rather than present a premature or thinly supported treatment alongside the two structurally and experimentally more established families that form the core, 102-page scope of this review.

On quantitative entropy–property relationships: We would like to draw the reviewer's attention to Section 4.4 ("Bridging Synthesis Pathway and Magnetic Outcome") and the accompanying quantitative benchmarking table, both of which were developed specifically to move the manuscript beyond qualitative description toward an explicit, mechanism-resolved treatment connecting configurational entropy, synthesis route, and realized magnetic parameters (Ms, Hc, Tc). We believe this directly addresses the reviewer's concern that the stated aim of the review, elucidating how configurational entropy governs functional magnetic outcomes, is substantively fulfilled within the spinel and hexaferrite systems that constitute its scope.

On scientific novelty: We respectfully note that a review article's contribution is conventionally judged by the quality of its critical synthesis rather than by the presentation of new experimental data. We believe this manuscript's value lies precisely in unifying a fragmented and rapidly growing literature into a coherent structure–synthesis–property framework, in critically comparing synthesis routes and their consequences for magnetic behavior, and in identifying concrete, underexplored directions for the field including the emerging role of garnet ferrites, which we now discuss explicitly as a future direction rather than omit silently.

We thank the reviewer again for the depth of this evaluation, which has helped us better frame and justify the scope of the manuscript.