Dynamic covalent hydrogels are considered smart materials with a stimuli-sensitive nature and possessing great importance in biomedical applications. In the current work, a new hydrogel based on polylysine (PLL), cellulose nanowhisker dialdehyde (DACNW), and chitosan (Cs) containing pH-sensitive dynamic covalent imine bonds was synthesized and along with its synthesis its potential application in curcumin (CUR) delivery was studied. Also, the antibacterial activities of hydrogel and drug-loaded hydrogels were evaluated. The prepared hydrogel also was characterized using techniques such as XRD, UV-VIS, FE-SEM, TGA, FT-IR and H-1-NMR spectroscopy. The resulting hydrogel showed excellent pH dependent curcumin delivery. Moreover, curcumin-loaded hydrogel showed good antibacterial activity against both Gram-negative and Gram-positive bacteria. The resulting hydrogel due to its pH-sensitive imine bonds could be considered as smart anticancer drug carrier system with high antibacterial properties.