A commercial activated carbon that is based on coconut shell was modified to increase its mesopore size for the adsorption of albumin-bound bilirubin (AB bilirubin) and bilirubin. The characterization of activated carbon that was modified via liquid nitrogen adsorption indicated that its micropores were reduced in size and its mesopores enlarged. According to the adsorption kinetics results, its adsorption capacities for both AB bilirubin and bilirubin are substantially increased due to its enlarged mesopores. Along with the increased adsorption capacity, its adsorption rate to bilirubin is also substantially increased. The adsorption capacitiesfor bilirubin and AB bilirubin depend linearly on the cumulative mesopore volume in the size ranges of 2.4–4.1 nm and 8.0–30.0 nm, respectively. Additionally, bilirubin presents a faster adsorption rate than AB bilirubin.