Mucoadhesion can be exploited as a strategy to target drug and nutrient delivery to the outer mucosal layers of fish in aquaculture farms. Cellulose nanocrystals (CNC) derived from cellulose pulp fibers can interact with the mucosal membranes via hydrogen bonding, however, their mucoadhesive properties are weak and should be enhanced. In this study, CNC were coated with tannic acid (TA), a plant polyphenol with excellent wet-resistant bioadhesive properties, to strengthen their mucoadhesive capability. The optimal CNC:TA mass ratio was determined to be 20:1. The modified CNCs were 190 ± 40 nm in length and 21 ± 4 nm wide and displayed excellent colloidal stability, with a zeta potential of −35 mV. Turbidity titrations and rheological measurements revealed that the modified CNC possessed superior mucoadhesive properties compared to pristine CNC. Modification with tannic acid introduced additional functional groups for stronger hydrogen bond formation and hydrophobic interactions with mucin, which was confirmed by a large reduction in viscosity enhancement values in the presence of chemical blockers (urea and Tween80). The enhanced mucoadhesion of the modified CNC could be utilized for the fabrication of a mucoadhesive drug delivery system to promote sustainable aquaculture practices.