The enantiomers of a racemic photoresponsive material represent two distinct states that can be modulated with irradiation at a single wavelength by changing the handedness of the light, Dynamic control over molecular chirality was obtained by the interconversion of enantiomers of helically shaped molecules with either left or right circular polarized light (CPL). Photoresolution of the bistable compound as a dopant in a nematic liquid crystalline phase by CPL irradiation led to a chiral mesoscopic phase. The chiral information inherent to CPL is therefore transmitted to the bistable molecule, followed by amplification and macroscopic expression of the chirality.