The design of synthetic nanoparticles (NPs) capable of recognizing given chemical entities in a specific and predictable manner is of great fundamental and practical importance. Herein, we report a simple, fast, water-soluble, and green phosphine free colloidal synthesis route for the preparation of multifunctional enzyme-capped ZnS bionanocomposites (BNCs) with/without transitional metal-ion doping. The enzymes alpha-Chymotrypsin (CHT), associated with the NPs, are demonstrated as an effectual host for organic dye Methylene Blue (MB) revealing the molecular recognition of such dye molecules by the BNCs. An effective hosting of MB in the close proximity of ZnS NPs (with similar to 3 nm size) leads to photocatalysis of the dyes which has further been investigated with doped-semiconductors. The NP-associated enzyme alpha-CHT is found to be active toward a substrate (Ala-Ala-Phe-7-amido-4-methyl-coumarin), hence leads to significant enzyme catalysis. Irradiation induced luminescence enhancement (IILE) measurements on the BNCs clearly interpret the role of surface capping agents which protect against deep UV damaging of ZnS NPs.