Photocatalysis is an efficient and an eco-friendly way to eliminate organic pollutants from wastewater and filtration media. The major dilemma coupled with conventional membrane technology in wastewater remediation is fouling. In this study, the photocatalytic degradation potential of novel thermoplastic polyurethane (TPU) based NiO on aminated graphene oxide (NH2-GO) nanocomposite membranes was explored. The fabrication of TPU-NiO/NH2-GO membranes was achieved by the phase inversion method and analyzed for their performances. The membranes were effectively characterized in terms of surface morphology, functional group, and crystalline phase identification, using scanning electron microscopy, Fourier transformed infrared spectroscopy, and X-ray diffraction analysis, respectively. The prepared materials were investigated in terms of photocatalytic degradation potential against selected pollutants. Approximately 94% dye removal efficiency was observed under optimized conditions (i.e., reaction time = 180 min, pH 3–4, photocatalyst dose = 80 mg/100 mL, and oxidant dose = 10 mM). The optimized membranes possessed effective pure water flux and excellent dye rejection (approximately 94%) under 4 bar pressure. The nickel leaching in the treated wastewater sample was determined using inductively coupled plasma-optical emission spectrometry (ICP-OES). The obtained data was kinetically analyzed using first- and second-order reaction kinetic models. A first-order kinetic study was suited for the present study. Besides, the proposed membranes provided excellent photocatalytic ability up to six reusability cycles. The combination of TPU and NH2-GO provided effective strength to membranes and the immobilization of NiO nanoparticles improved the photocatalytic behavior.