In this work, a mesoporous activated carbon (AC) was prepared from a unique lignocellulosic biomass (water caltrop husk) in triplicate using a single-step physical activation process at lower temperature (i.e., 750 °C) and longer holding time (i.e., 90 min). Based on the pore properties and adsorption properties for removal of methylene blue (MB) as organic pollutant, the results proved that the resulting AC possesses a mesoporous feature with the Brunauer−Emmett−Teller (BET) surface area of 810.5 m2/g and mesopore volume of about 0.13 cm3/g. Due to its fast adsorption rate and maximal adsorption capacity fitted (126.6 mg/g), the mesoporous carbon material could be used as an excellent adsorbent for liquid-phase removal of MB. In addition, the pseudo-second-order model is well suited for describing the adsorption system between the cationic adsorbate and the resulting AC with oxygen surface groups.