In this research, the adsorption of gallium onto natural zeolite (clinoptilolite) and two mesoporous-activated carbons were compared and evaluated. The clinoptilolite was treated with HCl (HCPL), while mesoporous-activated carbons (MCSG60A and MCO1) were synthesized by replica method, using sucrose as the carbon precursor and silica gel as the template. These carbonaceous materials showed large pore sizes and mesoporous surface, as well as a suitable surface chemistry for cation adsorption, which promotes a high negative charge density. On the other hand, zeolites have narrower pore sizes, which hinders the material diffusion inside the particle; however, its strength is their ion exchange capacity. Regarding the gallium kinetic studies, it is described by Pseudo-second order model for both sorts of adsorbents. MCO1 is the best carbonaceous adsorbent studied, with a capacity of 4.58 mg/g. As for zeolites, between the two zeolites studied, HCPL showed the best results, with a gallium adsorption capacity of 3.1 mg/g. The gallium adsorption mechanism onto MCO1 material is based on physisorption, while HCPL is mainly retained due to an ion-exchange process. Regarding the Giles classification, MCO1 isotherm described an H-4 pattern of high affinity and characteristic of multilayer adsorption. The Double-Langmuir model fits properly within these experimental results. In the case of zeolites, HCPL adsorption isotherm followed an L-2 pattern, typical of monolayer adsorption—the Sips model is the one that better describes the adsorption of gallium onto the zeolite.