Exploring Geometric Chirality in Nanocrystals for Boosting Solar‐to‐Hydrogen Conversion

Abstract Advancing catalyst design is pivotal for the enhancement of photocatalytic processes in renewable energy conversion. The incorporation of structural chirality into conventional inorganic solar hydrogen nanocatalysts promises a significant transformation in catalysis, a feature absent in this field. Here we unveil the unexplored potential of geometric chirality by creating a chiral composite that integrates geometric chiral Au nanoparticles (NPs) with two‐dimensional C 3 N 4 nanosheets, significantly boosting photocatalytic H 2 evolution beyond the achiral counterparts. The superior performance is driven by the geometric chirality of Au NPs, which facilitates efficient charge carrier separation through the favorable C 3 N 4 ‐chiral Au NP interface and chiral induced spin polarization, and exploits high‐activity facets within the concave surfaces of chiral Au NPs. The resulting synergistic effect leads to a remarkable increase in photocatalytic H 2 evolution, with an apparent quantum yield of 44.64 % at 400 nm. Furthermore, we explore the selective polarized photo‐induced carrier separation behavior, revealing a distinct chiral‐dependent photocatalytic HER performance. Our work advances the design and utilization of chiral inorganic nanostructures for superior performance in energy conversion processes.