The pollution due to oil spills causes diverse problems such as water pollution, destruction of habitats, and health issues. An easy process to solve this problem is fabricating hydrophobic sorbents. Metal-organic frameworks (MOFs)@polyurethane (PU) sponges in 3D structures are promising candidates to remove pollutants through sorption due to their intrinsic characteristics of MOFs and PU sponges, including porosity, low density, and mechanical strength. In this research, some novel MOFs@PU sponges were fabricated by incorporating MIL-101(Cr) or octadecylamine (ODA)-modified MIL-101(Cr), m-MIL-101(Cr), into PU sponges using PDMS (polydimethylsiloxane) as an adhesive agent. The prepared materials were investigated by various techniques including Fourier transform infrared (FT-IR), x-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive x-ray (EDS) mapping, water contact angle (WCA), and BET (Brunauer–Emmett–Teller) analyses. The WCA increased from 106.36° for the pristine PU to 145.06° and 157.98° for the as-prepared MIL-101(Cr)@PU and m-MIL-101(Cr)@PU, respectively. The uptake efficiency of the as-obtained sorbents for some oils (olive oil, sesame oil, sunflower oil, hydraulic oil, and diesel) and organic solvents (toluene, dichloromethane, ethyl acetate, chloroform, and n-hexane), as well as the ability of the m-MIL-101(Cr)@PU sponge for separation of diesel oil, chloroform, and toluene from water, were studied. The maximum sorption capacity was 79.83 g g−1 and 97.50 g g−1 for sesame oil and chloroform, respectively, using m-MIL-101(Cr)@PU as sorbent, which was higher than the efficiency of the pristine PU adsorbent. Additionally, the m-MIL-101(Cr)@PU sponge composite exhibited proper reusability of up to 7 cycles (∼52.88 g g−1). Overall, the as-obtained m-MIL-101(Cr)@PU sorbent exhibits promising potential to uptake oil and organic solvent contaminants.