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Hydrogels have gained significant attention in scientific communities for their versatile applications, but several challenges need to be addressed to exploit their potential fully. Conventional hydrogels suffer from poor mechanical strength, limiting their use in many applications. Moreover, the crosslinking agents used to produce them are often toxic, carcinogenic, and not bio-friendly. This study presents a novel approach to overcome these limitations by using bio-friendly modified nanocrystalline cellulose as a crosslinker to prepare highly stretchable and tough thermosensitive hydrogels. The surface of nanocrystalline cellulose was modified with 3-methacryloxypropyltrimethoxysilane (MPTS) to obtain modified nanocrystalline cellulose (M-NCC) crosslinker and used during free radical polymerization of thermosensitive N -isopropyl acrylamide (NIPA) monomer to synthesize NIPA/M-NCC hydrogel. The resulting nanocomposite hydrogels exhibit superior mechanical, thermal, and temperature-responsive swelling properties compared to conventional hydrogels prepared with traditional bi-functional N , N '-methylene bis (acrylamide) (MBA) as a crosslinker. The elongation at break, tensile strength, and toughness of the NIPA/M-NCC hydrogels significantly increase and Young's modulus decrease than conventional hydrogel. The designed M-NCC crosslinker could be utilized to improve the mechanical strength of any polymeric elastomer or hydrogel systems produced through chain polymerization., (© 2023 IOP Publishing Ltd.)