Chiral photocatalytic nanomaterials possess numerous unique properties and hold promise for various applications in chemical synthesis, environmental protection, energy conversion, and photoelectric devices. Nevertheless, it is uncommon to develop effective means to enhance the asymmetric catalytic performances of chiral plasmonic nanomaterials. In this study, a type of L/D‐Au@CeO2 helical nanorods (HNRs) was fabricated by selectively growing CeO2 on the surface of Au HNRs via a facile wet‐chemistry construction method. Chiral Au@CeO2 HNRs, featuring Au and CeO2 with spatially separate structures, exhibited the highest photocatalytic performance for N2 fixation, being 50.80 ± 2.64 times greater than Au HNRs. Furthermore, when L‐Au@CeO2 HNRs corresponded left circularly polarized light (CPL) and D‐Au@CeO2 HNRs corresponded right CPL, their photocatalytic efficiency was enhanced by 3.06 ± 0.06 times in contrast with the samples illuminated with the opposite CPL, which can be attributed to the asymmetrical generation of hot carriers upon CPL excitation. This study not only offered a simple approach to enhance the photocatalytic performance of chiral plasmonic nanomaterials but also demonstrated the potential of chiral plasmonic materials for application in specific photocatalytic reactions, such as N2 fixation.
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