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Air pollution is related to the development of the national economy and people’s livelihoods. Formaldehyde, as one of the main pollutants in the air, affects people’s physical and mental health. In order to remove formaldehyde and better protect the health of residents, it is necessary to develop efficient adsorption materials. In this study, APMDS-modified cellulose composite aerogel microcrystalline was investigated. The adsorption of formaldehyde by the MCC/APMDS (Microcrystalline Cellulose/N-(2-aminoethyl)-3- Aminopropyl Methyl Dimethoxysilane) composite aerogel mainly relied upon the reaction of the protonated –NH3+ group in APMDS with formaldehyde to form a Schiff base to achieve the effect of deformaldehyde. Meanwhile, the modification of the aerogel reduced the pore volume and specific surface area, and the average pore size increased to 14.56 nm, which enhanced the adsorption capacity of formaldehyde, and the adsorption amount reached 9.52 mg/g. This study provides valuable information for the preparation of adsorbent materials with high formaldehyde adsorption capacity for air purification.