The insufficient photosensitivity of conventional organic recording materials such as phenanthraquinone-doped poly(methyl methacrylate) (PQ/PMMA) significantly limits the recording speed in holographic data storage. Accelerating the formation of free radicals using the photosensitizer PQ during the photoreaction process and increasing the C = C double bond concentration of the matrix are effective methods for improving the photosensitivity. Using the above methods, we doped PQ/PMMA with the co-photoinitiator triethanolamine and co-monomer acrylamide to improve the photosensitivity of the material. Compared with the original PQ/PMMA material, the photosensitivity was increased by 10 times, and the diffraction efficiency was increased by 20%. The role of each doping component was studied by characterization and analysis. In addition, the introduction of the cross-linking agent N,N'-methylene-bisacrylamide, having high sensitivity, reduced the shrinkage of the material. We verified the application of the new material in a collinear system, and its high sensitivity showed its great potential for holographic data storage.