In this research study the potential of date palm leaves as an efficient biosorbent to adsorb crystal violet as one of the toxic cationic dyes from aqueous solution was investigated. Date palm leaves were characterized by SEM-EDX, BET, and FT-IR. The influence of prominent parameters such as pH, temperature, time, initial dye concentration, and amount of biosorbent on the removal (%) were studied using central composite design (CCD). RSM modeling was utilized to state the removal (%) as a function of the studied experimental parameters. Two statistical approaches were employed to develop RSM models: stepwise selection and ant colony optimization (ACO). Using another ACO algorithm, the best obtained operational conditions were 10.10, 55.92 °C, 21.10 min, 16.35 mg L−1, and 48.64 mg for pH, temperature, time, initial dye concentration, and biosorbent amount, respectively. The final results confirmed higher capability and accuracy of ACO-RSM in prediction compared with stepwise-RSM with shorter equation phrases. Maximum adsorption percent of 99.5 ± 0.4 predictably and 99.1 ± 0.1 experimentally were achieved under the optimal conditions. The experimental data were found to be suitably fitted to the Freundlich model with maximum adsorption capacity of 37.736 mg g−1.