Comprehensive SummarySensing the chirality of molecules is of great importance to fields such as enantioselective synthesis, pharmaceutical industry, and biomedicine. Plasmonic nanoparticles are ideal candidates for molecular sensing due to their inherent plasmonic properties that significantly enhance their sensitivity to surrounding molecules. Developing plasmonic nanoparticle‐molecule complexes for chirality sensing has drawn enormous attention in recent years due to their intriguing properties and potential applications. Thus, in this review, we believe it is timely to circumnavigate the rational design of plasmonic nanoparticle‐molecule complexes and widen the scope of their emerging applications in chirality sensing. First, we present different fundamental mechanisms for plasmon‐based chirality that are built on the system of plasmonic nanoparticle‐molecule complexes. Second, we review the typical applications of plasmonic nanoparticle‐molecule complexes in chirality sensing. Third, we discuss the emerging biomedical applications that the plasmon‐based chirality has attracted enormous interest. Finally, we provide an outlook on the challenges and opportunities in the field of plasmonic approaches for chirality sensing.This article is protected by copyright. All rights reserved.