The recent interest in the adsorption of pollutants on biomaterials has been gaining widespread attention, especially in the utilization of natural materials of vegetable origin-based composite biomaterials. In this study, the equilibrium and the kinetics of Crystal Violet adsorption onto native Carpobrotus edulis Mediterranean plant, which is biodegradable and less expensive, was investigated. Experiments were carried out as a function of adsorbent dose (0.08–1 g), contact time initial (5–180 min), ionic strength of salt NaCl (0.05–0.5 M), and solution pH (2–12). pH and ionic strength do not have a major influence on the adsorption of Crystal Violet on the biomaterial studied. The adsorption process followed a kinetic model of the pseudo-second-order. These results suggest that the native Carpobrotus edulis plant could potentially be used as an environmentally friendly adsorbent for eliminating cationic dyes from aqueous solutions.