The highly efficient, pollution-free and degradable biomass-based adsorbents used for the purification of wastewater are currently being highlighted in the research. Bamboo is an excellent raw material for pulp production due to its characteristics of fast growth, wide distribution and high cellulose content. In this study, a tannin/chitosan/bamboo pulp aerogel (TCPA), an environmentally friendly, renewable and low-density adsorbent, was synthesized using a simple freeze-drying method and analyzed by FTIR, XPS, SEM, TEM, TGA and surface area and porosity methods. TCPA has a large specific surface area (137.33 m2/g) and 3D porous structure, and its surface has multiple functional groups including amino, carboxyl and hydroxyl groups, which lead to a simultaneous absorption effect with Me2+ (Cu2+ and Cd2+). The maximum adsorption capacity for Cu2+ and Cd2+ of the TCPA was 72.73 mg/g and 52.52 mg/g, respectively. The adsorption processes of Me2+ by TCPA follow the pseudo-second-order model and Langmuir isotherm mode, and the adsorption processes are spontaneous and endothermic. The study provides a promising candidate for the treatment of wastewater containing heavy metal mixtures.