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To exploit the near-infrared (NIR) light of MoO₃, the MoVO_x mixed oxide was synthesized using a one-pot approach. The effects of different electrodes, V doping, and bias on the optoelectronic properties were investigated. The photoelectric responses to light sources with wavelengths of 405, 532, 650, 780, 808, 980, and 1064 nm were studied using both Au and carbon electrodes with 6B pencil drawings. The results demonstrate that the MoVO_x nanoblets exhibit photocurrent switching characteristics across the broadband region of the light spectrum. Even when zero bias was applied and the mixed oxide sample was stored at room temperature for over two years, a good photoelectric signal was still observed. This demonstrates that the MoVO_x nanoblets present an interface where interfacial charge transfer forms a strong built-in electric field, promoting photogenerated charge separation and transfer while suppressing photogenerated carrier recombination, and exhibiting self-powered characteristics. Interestingly, reducing the power of the typical excitation light sources resulted in a transition from positive to negative photocurrent features. This reflects the result of an imbalance between the concentration of material defects and the concentration of photogenerated electrons. The MoVO_x nanoblets not only enhance charge transport performance, but also significantly improve the exploitation of near-infrared light. Doping with V significantly improves the nanocomposites’ near-infrared (NIR) photoelectric sensitivity. This study demonstrates that heavily doping aliovalent ions during the in situ preparation of nanocomposites effectively enhances their photophysical properties. It provides a straightforward approach to narrowing the band gap of wide-bandgap oxides and effectively avoiding the recombination of photogenerated carriers. Full article