Oil/water separation is a field of high significance as it might efficiently resolve the contamination of industrial oily wastewater and other oil/water pollution. In this paper, an environmentally-friendly hydrophobic aerogel with high porosity and low density was successfully synthesized with renewable pomelo peels (PPs) as precursors. Typically, a series of sponge aerogels (HPSA-0, HPSA-1 and HPSA-2) were facilely prepared via high-speed dispersion, freeze-drying and silanization with methyltrimethoxysilane. Indeed, the physical properties of aerogel such as density and pore diameter could be tailored by different additives (filter paper fibre and polyvinyl alcohol). Hence, their physico-chemical properties including internal morphology and chemical structure were characterized in detail by Fourier transform infrared, Brunauer–Emmett–Teller, X-ray diffraction, scanning electron microscope, Thermal gravimetric analyzer (TG) etc. Moreover, the adsorption capacity was further determined and the results revealed that the PP-based aerogels presented excellent adsorption performance for a wide range of oil products and/or organic solvents (crude oil 49.8 g g −1 , soya bean oil 62.3 g g −1 , chloroform 71.3 g g −1 etc.). The corresponding cyclic tests showed the absorption capacity decreased slightly from 94.66% to 93.82% after 10 consecutive cycles, indicating a high recyclability.