The development of a bio-inspired method to fabricate ZnO nanostructure-modified functional wool fabric represents a substantial challenge in the textile field. This article reports for the first time the use of wool as a reducing agent for the synthesis of ZnO nanoparticles. While previous studies have employed alternative natural reducing agents for surface modification of host materials, this investigation uniquely utilizes the host material, wool, as the reducing agent for in-situ ZnO nanoparticle synthesis. In addition to demonstrating the use of wool as a reducing agent, this literature uniquely reports the durability of the modified fabric, achieved through the use of trimethoxy methyl silane. This silane compound acts as a bridging agent, forming a strong interface between the wool fibers and the synthesized ZnO nanoparticles. This innovative approach enhances the adhesion and stability of the ZnO nanoparticles on the wool fabric, a key aspect that contributes to the overall durability and performance of the modified material. The in situ surface modification process employed a metal oxide precursor (zinc acetate dihydrate), capping agents (hexamethylene tetraamine, sodium carbonate, and sodium sulfate), and a coupling agent (trimethyl methoxy silane). The capping agents were used to control the reaction conditions, while the coupling agent was employed to improve the durability of the surface modification. The impact of three different capping agents on the corresponding synthesis process was assessed, and the findings revealed that the choice of capping agent helped to form ZnO nanoparticles with distinct morphologies. Analytical techniques, such as X-ray diffraction (XRD), scanning electron microscopy (SEM), dynamic light scattering (DLS), and attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy, were utilized to characterize the synthesized particles and the treated fabric. The XRD analysis coupled with SEM analysis confirmed the successful formation of ZnO nanoparticles. The ATR-FTIR spectroscopy provided evidence of the formation of Si-O-Zn and Si-O-C bonds, observed at around 920 cm−1 and 1040 cm−1 respectively. These spectroscopic findings indicate that the surface modification involving the silane compound has enhanced the durability of the ZnO-modified fabric. The covalent linkages between the ZnO nanoparticles, the silane compound, and the wool fibers, confirmed by SEM analysis before and after washing cycles, have enabled the durable attachment of the nanoparticles to the fabric surface, even after multiple washing cycles. The results suggest a novel pathway to use wool as a reducing agent for the surface modification of the same material. Detailed mechanistic insights into the surface modification process and the corresponding chemical interactions were also discussed.