The effective disposal of redundant tea waste is crucial to environmental protection and comprehensive utilization of trash resources. In this work, the removal of methyl orange (MO) from aqueous solution using spent tea leaves as the sorbent was investigated in a batch experiment. First, the effects of various parameters such as temperature, adsorption time, dose of spent tea leaves, and initial concentration of MO were investigated. Then, the response surface methodology (RSM), based on Box–Behnken design, was employed to obtain the optimum adsorption conditions. The optimal conditions could be obtained at an initial concentration of MO of 9.75 mg·L^-1, temperature of 35.3°C, contact time of 63.8 min, and an adsorbent dosage 3.90 g·L^-1. Under the optimized conditions, the maximal removal of MO was 58.2%. The results indicate that spent tea leaves could be used as an effective and economical adsorbent in the removal of MO from aqueous solution.