Despite the recent advancement in graphene oxide (GO) as a host material in energy and environmental sectors, its composite thin films with metal oxides such as nickel oxide (NiO) and its optical, structural, chemical state, and photocatalytic activities have been poorly explored. Herein, we have reported the GO/NiO thin films preparation by a combination of chemical and physical deposition techniques (i.e. spin coating followed by DC/RF sputtering). The as-prepared composites thin films were characterised using Raman spectroscopy, X-ray diffraction/photoelectron spectroscopy scanning electron microscopy, and atomic force microscopy. The surface topography confirmed the uniform deposition of NiO over thin films of GO. The XPS results showed the formation of NiC along with the partial reduction in GO into graphene with their existing four constituents, i.e. NiO, NiC, GO, in the thin film composites. The classical plasmon, Wemple and Didomenico model, was first time applied for GO/NiO to compute energy loss functions, and dispersion energy parameters. The theoretical calculated values for the deposited GO/NiO thin films were found to be in very close agreement to the standard classical plasmon values. The change in spin orbital movement of Ni is considered due to the interaction between its nanoparticles and basal planes of GO. Thin films applied for the photodegradation of recalcitrant organic pollutant 2-chlorophenol (2-CP) revealed the dependence of photocatalytic efficiency on particle size and also on the interaction of GO with NiO rather than the ratio of NiO and GO in the films.