As an environmentally friendly material, graphene aerogel has been widely studied. The photothermal conversion performance is an important property of graphene aerogel. Graphene aerogels were prepared by hydrothermal reduction method. The factors affecting its surface photothermal conversion properties were explored and graphene aerogels with ideal photothermal conversion properties were obtained. In addition, COMSOL Multiphysics simulation was carried out to further analyze the intrinsic factors affecting the photothermal properties of the materials. The prepared materials were characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and Raman spectrometry (Raman) to obtain their physicochemical properties. UV–visible-near infrared spectrophotometer and microcomputer-controlled electronic universal testing machine were used to evaluate the light-absorbing capacity and mechanical properties of the materials. The obtained graphene aerogel can be rapidly heated up to higher than 110 °C in 8 s on its surface under simulated sunlight (1000 W·m−2) irradiation. When used for the treatment of oil spill at sea, the prepared graphene aerogel with good photothermal conversion ability can adsorb 105.61 times of its own weight of crude oil and the adsorption rate is as high as 10.56 g·g−1·min−1, which shows a broad application prospect.