Photoelectric properties of heterostructures consisting of deposited films of an inorganic semiconductor (IS) - CdSSe or molecular crystals (MC) with different molecular structure (phthalocyanines of Pb, ClAlCl) and nematic liquid crystal BL055 have been studied. The main attention was given to the: effect of MC molecular structure on the creation of potential barriers at MC/LC interface in heterostructures and effect of them on processes of polarization by strong absorbed light excitation and external constant electric field of different polarity.