Metal-organic framework (MOF) structures containing different metal ions and 1,3,5-trimesic acid (BTC) were fabricated, as the carriers to immobilize chitinase (Chi) for improving the performance of Chi, for the first time. It was found that the immobilization of Chi on Ca-BTC, Ba-BTC, and Ni-BTC increased its activity. Notably, the specific activity of Chi@Ca-BTC was enhanced by 2.1 times that of free Chi, reaching 16.27 U/mg. The catalytic efficiency and substrate affinity of Chi@Ca-BTC were also remarkably improved, confirmed by the k