Development of absorbent material for oil and organic solvents is critical for removing contaminants from the water surface. Advancement of an oil absorber with a significant contribution for structural parameters of porous configuration of materials is highly coveted in order to ensure crude oil supply for future generations. In this study, we demonstrate structural parameters of the pores of surface modified two-dimensional (2D) CuSe nanoflakes engineered polyurethane (PU) sponge, with combination of synergistic low surface energy and surface roughness, playing an important role in the efficient removal of oil from water. Due to large surface of porous sponge and two dimensional nanoflakes along with their interface, the system showed an efficient crude oil uptake capacity of more than 37 times of its original mass. Furthermore, the developed system can be recycled and reused 50 times while maintaining high crude oil absorption efficiency, and even after 50 cycles, the system has retained good recycling absorption capacity, indicating the brilliance of the system. In addition, the system has promising implications as a favorable absorbent for crude oil–water separation due to its quick absorption (1.5 s) and high separation efficiency (96%). The selective absorption efficiency, quick oil-absorption rate, large amount of oil separation with high efficiency under one platform, has been implemented in a device for technological application in large scale.