This article focuses on silanisation of reinforcement surfaces to improvise reinforcement-matrix interfaces for developing nettle/PLA biocomposites with enhanced mechanical, thermo-mechanical, and biodegradation properties. Two different silane coupling agents, namely Tri-ethoxy silyl propyl methacrylate (TES-PM) and Amino propyl tri-ethoxy silane (APTES) are taken at different levels of concentration and grafted on the surface of cellulosic nettle reinforcement. The degree of silanisation is measured as an evidence of successful coupling reaction determining the morphological, structural, chemical and mechanical characteristics of the nettle woven reinforcement. It is shown that the interfacial strength of the biocomposite depends on the functional moiety and the level of concentration of the silane coupling agents. It is demonstrated that an appropriate silane coupling agent with an optimal level of concentration brings forth substantial improvement in the static mechanical (tensile, flexural and impact), dynamic mechanical (storage & loss moduli and damping factor) and biodegradation properties of nettle/PLA biocomposite without significant change in the thermal properties.