The process of washing and removing crude oil from spent catalysts is a serious issue in both catalyst regeneration and precious metals recovery. In this work, five different solvents with various polar and aromatic properties were chosen to evaluate their impact on the catalyst support structure and crude oil recovery from oil-contaminated spent catalysts. After the deoiling process, the spent catalyst was analyzed by scanning electron microscopy, X-ray diffraction (XRD), Fourier transform-infrared spectroscopy, elemental analyzer, contact angle measurement, gas chromatography-mass spectrometry, inductively coupled plasma-atomic emission spectroscopy, and Brunauer Emmet Teller (BET) method. Our findings demonstrate that p-xylene and kerosene are more effective in removing oil than other solvents. This is due to crude oil’s similar polarity and molecular nature with kerosene and p-xylene. Considering the economical reason, kerosene is a better choice for deoiling spent catalyst compared to p-xylene as it is more affordable than p-xylene. XRD data show that the structure of the catalyst support was unaltered by the solvent treatment process, while BET data reveals that the surface area and pore volume are significantly enhanced after the deoiling process. These results imply that deoiling is a very crucial step for the recycling, regeneration, and reuse of spent catalysts. Our work is significant in developing sustainable approaches for managing spent catalysts, and minimizing waste and environmental pollution.