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Construction materials and techniques have witnessed major advancements due to the application of digital tools in the design and fabrication processes, leading to a wide array of possibilities, especially in additive digital manufacturing tools and 3D printing techniques, scales, and materials. However, possibilities carry responsibilities with them and raise the question of the sustainability of 3D printing applications in the built environment in terms of material consumption and construction processes: how should one use digital design and 3D printing to achieve minimum material use, minimum production processes, and optimized application in the built environment? In this work, we propose an optimized formal design of “Biodigital Barcelona Clay Bricks” to achieve sustainability in the use of materials. These were achieved by using a bottom-up methodology of biolearning to extract the formal grammar of the bricks that is suitable for their various applications in the built environment as building units, thereby realizing the concept of formal physiology, as well as employing the concept of fractality or pixilation by using 3D printing to create the bricks as building units on an architectural scale. This enables the adoption of this method as an alternative construction procedure instead of conventional clay brick and full-scale 3D printing of architecture on a wider and more democratic scale, avoiding the high costs of 3D printing machines and lengthy processes of the one-step, 3D-printed, full-scale architecture, while also guaranteeing minimum material consumption and maximum forma–function coherency. The “Biodigital Barcelona Clay Bricks” were developed using Rhinoceros 3D and Grasshopper 3D + Plugins (Anemone and Kangaroo) and were 3D printed in clay. Full article