By employing film-forming polymer with low molecular weights, supplementary monomers and different photosensitive reagents, a green sensitive polyvinyl alcohol/acrylamide based photopolymer with high diffraction efficiency and photosensitivity is reported, the absorption spectra, the effects of dye concentration and film thickness on diffraction efficiency and photosensitivity are studied systematically. Diffraction efficiency higher than 82% is obtained at the exposure level of 20 mJ/cm2, maximum diffraction efficiency can reach to 92%. Furthermore, the angular selectivity of the photopolymer is also tested and its corresponding Bragg selective angle width is 0.57°. The preliminary applications of angular and spatial multiplexing holographic storage are also demonstrated, bright and distinct holographic storage samples are obtained readily.