Polyprolylene is commonly used for crude oil spill cleaning, but it has low absorption capacity and is nonbiodegradable. In our work, a green, ultralight, and highly porous material was successfully prepared from paper waste cellulose fibers. The material was functionalized with methyltrimethoxysilane (MTMS) to enhance its hydrophobicity and oleophilicity. Water contact angles of 143 and 145° were obtained for the MTMS-coated recycled cellulose aerogel. The aerogel achieved high absorption capacities of 18.4, 18.5, and 20.5 g/g for three different crude oils at 25 °C, respectively. In the investigated temperature range of 10, 25, 40, and 60 °C for the absorption of the tested crude oil on the aerogel, a highest absorption capacity of 24.4 g/g was obtained. It was found that the viscosity of the crude oils is the main factor affecting their absorption onto the aerogel. The strong affinity of the MTMS-coated recycled cellulose aerogel to the oils makes the aerogel a good absorbent for crude oil spill cleaning.