Microcrystalline cellulose (MCC) aerogels were synthesized, blendingwith high amylose corn starch of different contents based on a NaOH–urea solution, and following by vacuum freeze-drying technology. The microstructure of the aerogel was observed by scanning electron microscopy (SEM) as an interconnected, porous three-dimensional structure, while X-ray diffractogram (XRD) measurements showed that the crystalline form was converted from cellulose I to cellulose II during dissolution and regeneration. Thermogravimetric analysis (TGA) showed that the content of starch had little effect on the thermal stability of the aerogel, whereas the content of starch had great influences on absorption and viscoelastic properties. When the ratio of starch was 10% and 15%, the prepared aerogels presented a low density and abundant pores, which endowed the aerogels, not only with the highest absorption ratio of pump oil and linseed oil (10.63 and 11.44 g/g, respectively), but also with better dynamic viscoelastic properties.