We furnish a comprehensive study on light-induced carrier generation due to the synergistic contribution of Au interband transition and graphene oxide (GO)/ZnO heterostructure. Plasmonic gold nanoparticles (Au_nps) are incorporated as a substructure sandwiched between GO and ZnO, assisting in additional photo-induced charge carrier generation. GO is prepared by a single-step plasma-enhanced chemical vapor deposition process. The GO/ZnO heterostructure having an active working area of 0.25 cm2 is created to unleash the pyroelectric property of ZnO, and subsequently, Au_np is introduced at the interface of GO/ZnO. Here, the interband transition of Au_np and its capability for charge carrier generation combined with the excitonic charge carrier generation of the highly crystalline non-centrosymmetric hexagonal wurtzite ZnO enhances the photoresponse. Furthermore, the interaction of Au_np with ZnO and its spatial electric field intensity distribution is demonstrated by finite difference time domain simulation which indicate toward an efficient carrier generation at the interface of Au_np and ZnO. The fabricated heterostructure has an active working wavelength in the UV-A region with the highest responsivity at 375 nm of the electromagnetic spectrum. The ultrafast response time (∼29 μs) of the device is due to the pyro-phototronic effect of the GO/ZnO heterostructure enhanced by the interband transition of Au. In the comparative study of the Au_np-enriched GO/ZnO heterostructure device with a GO/ZnO device, the former shows better performance. Both the devices work in the self-powered mode as well as the photoconductive mode, but with a higher on–off current ratio in the photoconductive mode. Hence, this work helps in properly understanding photo-induced charge generation in a Au interband transition enriched GO/ZnO heterostructure.