•The compounded MCC/PDA aerogels were prepared.•Morphology and microstructure of the aerogel was tailored by changing PDA content.•The aerogel showed high adsorption ability and excellent adsorption selectivity. As one of the materials from natural resources, the functionalization and application of cellulose attract increasing concerns. In this work, we reported a facile method to prepare the bio-inspired functionalization of microcrystalline cellulose (MCC) aerogel through polydopamine (PDA) coating, which was realized via the self-polymerization of dopamine in the MCC/LiBr solution followed by the freeze-drying technology. The morphological characterization showed that the pore morphologies of the compounded aerogel were influenced by the content of PDA. Adsorption measurements toward methylene blue (MB) showed that the compounded aerogel had high adsorption ability. Moreover, the compounded MCC/PDA aerogel exhibited excellent adsorption selectivity and it exhibited high efficiency to remove MB from different solutions, such as the mixed solution with anionic dyestuffs, the mixed solution with cationic dyestuffs and the mixed solution with common salt (NaCl). The high adsorption ability and excellent adsorption selectivity endows the compounded MCC/PDA aerogel with great potential applications in wastewater treatment.