Abstract Chiral plasmonic nanostructures have attracted increasing attention because of their superchiral near‐fields as well as strong far‐field chiral optical response. Recently, the development of chemical synthesis methods enabled the large‐scale manufacturing of three‐dimensional colloidal chiral plasmonic nanocrystals. Further improving the chiral optical response of such nanostructures will greatly facilitate their practical applications. In this work, it is found both in calculations and experiments that chiral cavity plasmon resonances can be excited in film‐coupled chiral Au helicoid nanoparticles, enabling the significant enhancement of the nanostructure chiral optical response. In addition, it is demonstrated from simulation that the chiral cavity mode can modulate the emission polarization of a point electric dipole placed in the nanocavity formed by the nanoparticle and the Au film, allowing the emission of almost circularly polarized photons by the linear dipole with the emission circular polarization anisotropy factor reaching as high as 93%. The film‐coupled chiral plasmonic nanoparticles therefore provide a promising platform for the construction of advanced chiral optical devices such as on‐chip nonreciprocal nanoscale light sources, chiral plasmonic sensors, chiral metamaterials, plasmonically enabled valleytronic devices, and nanophotonic circuits for future on‐chip communication applications.