The controlled delivery of the desired bioactive molecules is required to achieve the maximum therapeutic effects with minimum side effects. Biopolymer-based hydrogels are ideal platforms for delivering the desired molecules owing to their superior biocompatibility, biodegradability, and low-immune response. However, the prolonged delivery of the drugs through biopolymer-based hydrogels is restricted due to their weak mechanical stability. We developed mechanically tough and biocompatible hydrogels to address these limitations using carboxymethyl chitosan, sodium alginate, and nanocellulose for sustained drug delivery. The hydrogels were cross-linked through calcium ions to enhance their mechanical strength. Nanocellulose-added hydrogels exhibited improved mechanical strength (Young's modulus; 23.36 → 30.7 kPa, Toughness; 1.39 → 5.65 MJm