Nanocomposites based on transparent polymer matrices containing nanoparticles (NPs) of noble metals are modern-day materials that can be specially designed for photonics, linear and nonlinear optics, laser physics and sensing applications. We present the improved photosensitive nanocomposites doped with Au and Ag NPs allowing fabrication of high effective submicrometer dimensional diffraction structures using holographic method. A general approach for the fabrication of holographic structures using a two-component mixture of the monomers of different reactivity was developed. Two different methods, ex situ and in situ, were studied to introduce Au and Ag NPs in the polymer matrix. The diffusion model of the grating formation upon holographic exposure as well as the process of Ag NP synthesis in a polymer matrix is considered. The influence of the NP size on the polymerization process, material dynamic range and nonlinear properties were investigated. The mechanisms and characteristics of the nanocomposite nonlinear optical response are discussed.