It is of great importance to develop cost-effective materials for large-scale use in CO2 capture and conversion. Herein, mesoporous N-doped carbon materials were prepared by one-step carbonization of tea waste (TW) in the absence of any other additives, and used as a class of bio-friendly adsorbents for CO2 capture and conversion. It is demonstrated that the as-prepared TW-derived N-doped carbon exhibit moderate CO2 adsorption capacities under 1 bar. They also display high activity for catalyzing the cycloaddition of CO2 with epoxides under mild conditions (e.g., 1 bar, 100 °C, and 8 h). Systematic characterizations prove that TW-900 shows moderate specific surface areas and superhydrophobicity feature, which are responsible for its high performance for CO2 capture and conversion. The direct carbonization of TW offers a facile and environmentally friendly route to N-doped carbon materials for CO2 capture and fixation.