This study investigates the feasibility of spent tea waste extract (STWE) as a green modifying agent for the modification of chitosan adsorbent towards aspirin removal. Response surface methodology based on Box-Behnken design was employed to find the optimal synthesis parameters (chitosan dosage, spent tea waste concentration, and impregnation time) for aspirin removal. The results revealed that the optimum conditions for preparing chitotea with 84.65% aspirin removal were 2.89 g of chitosan, 18.95 mg/mL of STWE, and 20.72 h of impregnation time. The surface chemistry and characteristics of chitosan were successfully altered and improved by STWE, as evidenced by FESEM, EDX, BET, and FTIR analysis. The adsorption data were best fitted to pseudo 2nd order, followed by chemisorption mechanisms. The maximum adsorption capacity of chitotea was 157.24 mg/g, as fitted by Langmuir, which is impressive for a green adsorbent with a simple synthesis method. Thermodynamic studies demonstrated the endothermic nature of aspirin adsorption onto chitotea.