Sustainability of the leather industry demands a paradigm shift from existing chemical-based processing to biobased degradable systems. Enzyme-based unhairing systems are evolving as an eco-friendly alternative to sodium sulfide-and limebased conventional unhairing process. However, factors such as uncontrolled enzyme activity over the skin thus resulting in poor quality of leather, cost, and poor recyclability limit their commercial exploitation. To overcome these challenges, herein, we synthesized zinc-based metal organic framework as a supporting matrix, immobilized the protease, and studied its efficiency and recyclability for unhairing of skins. ZnMOF and ZnMOF-protease (ZnMOF-Enz) were prepared and characterized by FTIR, DLS, XRD, XPS, HR-TEM, and FESEM analyses. The activity of the immobilized enzyme on ZnMOF was studied at different temperatures and pHs and optimized. The application of ZnMOF-Enz for unhairing of the goat skin was studied, and the hair removal efficiency was found to be efficient even after the four recycles with supplemented ZnMOF-Enz. The microscopic analysis results of the protease-treated and ZnMOF-Enz-treated skin reveal that the efficiency of ZnMOF-Enz was comparable to that of the protease-treated one even after a fourth cycle. The present study provides an insight into the usage of enzymes immobilized on MOFs as an alternative and sustainable approach for the unhairing process with a good recyclability factor.