In this study, we propose a facile in-situ approach to fabricate a silver (Ag) NPs decorated graphene oxide (GO) blended with glutaraldehyde (GA) crosslinked polyvinyl alcohol (PVA) matrix, resulting in a PVA/GO-Ag/GA nanocomposite. We investigated how gamma radiation affected the optical and electrical properties of the resulting nanocomposites. Our study reveals that exposure to gamma radiation decreases the band gap of PVA/GO-Ag/GA from 6.06 to 3.35 eV for a 2 kGy dose. The direct current (dc) electrical conductivity was measured to be 2.30 × 10−5 S cm−1 for a 2 kGy dose. Additionally, Jonscher's power law analysis of the alternating current (ac) conductivity behavior suggests that the conduction mechanism in the samples is most likely due to charge carrier transport after gamma irradiation. In conclusion, our findings demonstrate that irradiating PVA/GO-Ag/GA nanocomposites with gamma wavelengths yields tunable electrical and optical properties, making them potential candidates for optoelectronic and electromagnetic applications.