Circularly polarized light (CPL) with the end of optical vector traveling along circumferential trajectory shows left- and right-handedness, which transmits chiral information to materials via complicated CPL–matter interactions. Materials with circular dichroism respond to CPL illumination selectively with differential outputs that can be used to design novel photodetectors. Racemic or achiral compounds under CPL go through photodestruction, photoresolution, and asymmetric synthesis pathways to generate enantiomeric bias and optical activity. By this strategy, helical polymers and chiral inorganic plasmonic nanostructures are synthesized directly, and their intramolecular folding and subsequent self-assembly are photomodulable as well. In the aggregated state of self-assembly and liquid crystal phase, helical sense of the dynamic molecular packing is sensitive to enantiomeric bias brought by CPL, enabling the chiral amplification to supramolecular scale. In this review, the application-guided design strategies of CPL-responsive materials are aimed to be systematically summarized and discussed. Asymmetric synthesis, resolution, and property-modulation of small organic compounds, polymers, inorganic nanoparticles, supramolecular assemblies and liquid crystals are highlighted based on the important developments during the last decades. Besides, applications of light–matter interactions including CPL detection and biomedical applications are also referred.