We report on the fabrication of Glutaraldehyde (GA) crosslinked PVA/GO-Ag nanocomposite (PVA/GO-Ag/GA) via in situ thermal reduction. A careful and systematic investigation on PVA, PVA/GO, PVA-Ag, PVA/GO-Ag, and PVA/GO-Ag/GA nanocomposites has been explicitly conducted to exemplify the GA influence on enhancing the PVA/GO-Ag composite’s structural, optical, and functional properties. Finite Difference Time Domain (FDTD) simulations validate the experimental results by scrutinizing the compositional, morphological, and positional influence of Ag nanoparticles (NPs) in the polymer matrix in a systematic and comprehensive manner. The optical transmittance of PVA/GO-Ag/GA is enhanced up to 51 % (increased by ~ 89 %, 21 %, and 42 % of PVA/GO, PVA-Ag, and PVA/GO-Ag, respectively) due to the GA cross-linker. The band gap of PVA/GO-Ag/GA was found to be 5.289 eV, which is the lowest of the composites mentioned above. PVA/GO-Ag/GA exhibits enhanced dc conductivity of 17.3 × 10− 9 Sm− 1. Above measured values of transmittance, optical band gap, and electrical conductivity demonstrate that the fabricated GA crosslinked PVA/GO-Ag nanocomposite is an excellent candidate in terms of its applicability in multispectral imaging, optoelectronic, and optomechanical devices.