Nanocrystalline cellulose (NCC) is employed as the cross-linker and reinforcement domain for developing nanocomposite hydrogels possessing high strength and improved diffusion property; the resulting nanocomposite hydrogels are shown to have high mechanical properties, reversible swelling ability, and are biodegradable and biocompatible; the approach relies on free radical polymerization to form the hydrogels using a variety of hydrophilic vinyl monomers. These hydrogels are suitable for developing highly absorbent hygiene products, as well as for applications in medicine, engineering materials and sensors.