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Cellulose nanocrystals (CNCs) extracted from jute fibers are moderately high in length (up to 1200 nm) and diameter (up to 90 nm). Poly(N,N-dimethylacrylamide-co-3-methacryloxypropyltrimethoxysilane) (pSiDm) is a custom made copolymer with trimethoxy silane groups at one end which facilitates to react with cellulose in an aqueous solution. A very simple, efficient, rapid, and eco-friendly method was developed to prepare j-CNC reinforced pSiDm hydrogel to remove methylene blue (MB) dye from an aqueous solution. The reaction between j-CNCs and pSiDm in the hydrogel was revealed by the increased intensity ratio of –OH band to C–H band and shifting of a peak for C=O from 1604 cm−1 to 1608 cm−1 in the FT-IR spectrum of the hydrogel compared to those of the copolymer. Glass transition temperature of the copolymer increases from 99 to 111 °C after being applied into the hydrogel. The prepared hydrogel showed a significant swelling at a ratio of 16 g/g in deionized water. In good accordance with the Langmuir adsorption isotherm, a maximum adsorption value of MB onto the hydrogel was achieved 131.58 mg/g. Kinetic studies of the adsorption process fit well with a pseudo-second-order reaction model. The j-CNCs/pSiDm hydrogel is a moderately resilient and completely biodegradable material to be utilized for the adsorption of cationic toxic materials from waste effluent.