This work mainly focused on the preparation of a low-cost, ultralight absorbent from renewable corn straw and filter paper via a facile and environmental-friendly approach containing high-shear blending and freeze-drying operation. The physicochemical properties of aerogel were thoroughly examined by several characterization techniques. The satisfactory hydrophobicity of the spongy aerogel was attributed to the formation of polysiloxane on the surface of methyltrimethoxysilane (MTMS) by the silanization reaction. Owing to its superior features, such as ultralow density, high porosity, desirable hydrophobicity, the corn straw based spongy aerogel exhibited a remarkable absorption capacity for both crude oil (36 g/g) and common organic solvents including carbon tetrachloride (CCl4, 45 g/g), dimethyl sulphoxide (DMSO, 24 g/g), N, N-dumethylformamide (DMF, 45 g/g). This might shed light on the design of efficient adsorbent for oil spills and organic pollutants to meet with the sustainable development.