Organofunctionalized nanostructured silica SBA-15 with tri(2-aminoethyl)amine tetradentate-amine ligand was synthesized and applied as adsorbent for the removal of Cu2+, Pb2+, and Cd2+ from both synthetic wastewater and real paper mill and electroplating industrial effluents. The prepared materials were characterized by XRD, N2 adsorption-desorption, TGA, and FT-IR analysis. The Tren-SBA-15 was found to be a fast adsorbent for heavy metal ions from single solution with affinity for Cu2+, Pb2+, than for Cd2+ due to the complicated impacts of metal ion electronegativity. The kinetic rate constant decreased with increasing metal ion concentration due to increasing of ion repulsion force. The equilibrium batch experimental data is well described by the Langmuir isotherm. The maximum adsorption capacity was 1.85 mmol g−1 for Cu2+, 1.34 mmol g−1 for Pb2+, and 1.08 mmol g−1 for Cd2+ at the optimized adsorption conditions (pH=4, T=323 K, t=2 h, C0=3 mmol L−1, and adsorbent dose=1 g L−1). All Gibbs energy was negative as expected for spontaneous interactions, and the positive entropic values from 103.7 to 138.7 J mol−1 K−1 also reinforced this favorable adsorption process in heterogeneous system. Experiment with real wastewaters showed that approximately a half fraction of the total amount of studied metal ions was removed within the first cycle of adsorption. Hence, desorption experiments were performed by 0.3M HCl eluent, and Tren-SBA-15 successfully reused for four adsorption/desorption cycles to complete removal of metal ions from real effluents. The regenerated Tren-SBA-15 displayed almost similar adsorption capacity of Cu2+, Pb2+, and Cd2+ even after four recycles. The results suggest that Tren-SBA-15 is a good candidate as an adsorbent in the removal of Cu2+, Pb2+, and Cd2+ from aqueous solutions.