Hybrid perovskites have recently attracted enormous attention for photovoltaic applications, and various strategies related to light management and photocarrier collection are developed to enhance their performance. As an effective route toward near‐field light enhancement, metal nanostructures with subwavelength dimensions can couple incident photons with conduction electrons, giving rise to localized surface plasmon resonances. However, efficiency enhancements through plasmonic routes are limited to the short wavelength range corresponding to metal extinction wavelength. Thus, the exploration of novel plasmonic nanostructures with predesigned sizes and shapes is needed to advance this field. Herein, for the first time, a bioinspired nanostructure of Au nanorod–nanoparticle dimers with structural darkness is exploited to enhance the light harvesting and performance of perovskite solar cells. Differing from conventional metallic nanoparticles, biometric nanoparticles introduce geometric singularity to the system, providing a broadband response for energy harvesting. By embedding the core–shell gold dimers in the perovskite solar cells, a notable enhancement of broadband light absorption is observed, and sequentially, the efficiency of perovskite solar cells increases by 16%.
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