Although though ionic liquids (IL) are rapidly emerging as highly efficient reagents for the depolymerization of waste plastics, their high cost and adverse impact on the environment make the overall process not only expensive but also environmentally harmful. In this manuscript, we report that graphene oxide (GO) facilitates the transformation of waste polyethylene terephthalate (PET) to Ni-MOF (metal organic framework) nanorods anchored on reduced graphene oxide (Ni–MOF@rGO) through NMP (N-Methyl-2-pyrrolidone)-based coordination in ionic liquids. Morphological studies using scanning electron microscopy (SEM) and transmission electron microscopy (TEM) showed mesoporous three-dimensional structures of micrometer-long Ni-MOF nanorods anchored on reduced graphene substrates (Ni–MOF@rGO ), whereas structural studies using XRD and Raman spectra demonstrated the crystallinity of Ni-MOF nanorods. Chemical analysis of Ni–MOF@rGO carried out using X-ray photoelectron spectroscopy demonstrated that nickel moieties exist in an electroactive OH-Ni-OH state, which was further confirmed by nanoscale elemental maps recorded using energy-dispersive X-ray spectroscopy (EDS). The applicability of Ni–MOF@rGO as an electro-catalyst in a urea-enhanced water oxidation reaction (UOR) is reported. Furthermore, the ability of our newly developed NMP-based IL to grow MOF nanocubes on carbon nanotubes and MOF nano-islands on carbon fibers is also reported.