The synthesis of graphitic carbon nitride (g-C3N4) doped with s-block metals is described. The materials were synthesized via thermal polycondensation of cyanamide and the appropriate metal chloride. The inclusion of the metal precursor strongly influenced the surface chemistry features as well as the textural, morphological, and structural properties of the g-C3N4. The doping of g-C3N4 with s-block metals markedly enhanced its adsorption performance, which was studied during the removal of two model solutes (methyl blue and copper ions) from aqueous solutions. The maximum adsorption capacity for the organic dye was increased by 680 times after the doping process. The uptake of copper(II) increased ca. 30 times for the doped g-C3N4. The improvement of the adsorption performance is discussed in terms of the surface chemistry and textural features.