Volume holographic phase gratings possessing the saturated refractive index modulation amplitudes as large as 4.5×10-2 were recorded at a wavelength of 532 nm in a photopolymerizable nanoparticle-polymer composite (NPC) film dispersed with ultrahigh refractive index hyperbranched-polymer (HBP) organic nanoparticles. This prominent result was achieved by a combination of the HBP nanoparticles with triazine and aromatic ring units and an electron donor/acceptor photo-initiator system doped in an acrylate monomer blend with low viscosity. As a result, efficient mutual diffusion of HBP nanoparticles and monomer having their very large refractive index difference took place. Obtained results suggest a potentiality of our newly developed HBP-dispersed NPC gratings as efficient volume holographic optical elements for various photonic applications including wearable headsets for augmented and mixed reality.