Cyclosporine A (CsA), a naturally derived biomaterial and physiologically active substance, is commonly used as an immunosuppressant. In this study, CsA was revealed to function as a chiral inducer of cholesteric liquid crystals (CLCs) with a high helical twisting power. CsA induced helical structures in 4-cyano-4'-pentylbiphenyl, a synthetic liquid crystal (LC) used for general purposes. Electrochemical polymerization in CLC with CsA was also performed. The polymer prepared in CLC showed electro-optical activity via chiral induction by CsA. Synchrotron X-ray diffraction measurements indicated that the polymer film prepared in the CLC formed in the manner of LC molecular arrangement through molecular form imprinting from the LC order, although the polymer exhibited no liquid crystallinity. The polymer showed structural color and laser light oscillation diffraction derived from its periodic structure. The anisotropy of the circularly polarized electron spin resonance signals for the resulting polymer with respect to the magnetic field was observed.