Key Lab of Environment‐friendly Chemistry and Circularly polarized luminescent (CPL) materials with multitudinous inherent advantages shows extensive application. In this work, we prepare a kind of highly efficient wavelength‐tunable CPL free‐standing films by responsive chiral aggregation‐induced emission mesogen. Firstly, the pyridine‐functionalized tetraphenylethene monomer (MPy) is designed and synthesized. Then, the different ration of the monomer MPy mixed with the liquid crystal (LC) reactive monomer (LC242) to fabricate a free‐standing film by photopolymerization. The obtained film presents efficient CPL with a constant luminescence asymmetry factor (glum) of +0.75, as well as sensitive wavelength tunability. Finally, this wavelength‐tunable CPL film with both fluorescence and CPL modes is successfully applied in anti‐counterfeiting and information encryption. This work provides a simple way to construct CPL apparatus with adjustable luminescence wavelength and high glum.