Indoor formaldehyde from substandard furniture and decorative materials seriously endangers human health. How to remove effectively indoor formaldehyde with low concentration at room temperature is a challenging problem. Using a MnO2/AlOOH composite by the MnO2 modification as a catalyst provides an effective approach to solve this challenge. Here, a new type of MnO2/AlOOH composite catalyst with high ability to remove indoor low-concentration formaldehyde was prepared by redox reaction at room temperature. A MnO2/AlOOH composite with a homogeneous dispersion of MnO2 has high specific surface area and a large amount of surface hydroxyl (-OH) which plays a major role in the adsorption of formaldehyde. A partially crystalline structure was observed in the composite, which contains multivalent Mn ions and a large number of vacancy defects. The surface -OH of composite shows strong oxidation activity through the charge exchange of multivalent Mn ions and vacancy defects. The composite has a higher ability to remove indoor low-concentration formaldehyde compared to the birnessite MnO2 at room temperature. This study proposes a new idea for the improvement of catalytic performance in the structure and composition of the catalyst.