The optimization data presented here are part of the study planned to remove the caffeine from aqueous solution through the large surface area optimized H3PO4-activated Acacia mangium wood activated carbon (OAMW-AC). The maximum adsorption capacity of the OAMW-AC for caffeine adsorption was achieved (30.3 mg/g) through optimized independent variables such as, OAMW-AC dosage (3.0 g/L), initial caffeine concentration (100 mg/L), contact time (60 min), and solution pH (7.7). The adsorption capacity of OAMW-AC was optimized with the help of rotatable central composite design of response surface methodology. Under the stated optimized conditions for maximum adsorption capacity, the removal efficiency was calculated to be 93%. The statistical significance of the data set was tested through the analysis of variance (ANOVA) study. Data confirmed the statistical model for caffeine adsorption was significant. The regression coefficient (R2) of curve fitting through the quadratic model was found to be 0.9832, and the adjusted regression coefficient was observed to be 0.9675.