An efficient process was developed allowing the removal of metal ions from polycontaminated aqueous solutions by combining modified colloids and membranes. Firstly, filtration experiments were performed using polyethersulfone membranes modified by a self-assembled multilayer film of polyelectrolytes. These polymer-modified membranes allowed the uptake of more than 90% of the metal ions initially present in the contaminated solutions (for solutions concentrated at 50 mg L −1). Secondly, adsorption experiments were carried out with colloidal silica encapsulated with carboxymethyl chitosan (SiO 2-CMCS) or with mesoporous silica functionalized by grafting of 1,4,8,11-tetraazacyclotetradecane, i.e., cyclam (SiO 2-cyclam). The adsorption capacity of these compounds was shown to be higher than numerous other literature-known adsorbents, reaching 68 and 61 mg g −1 towards Cu(II) for SiO 2-CMCS and SiO 2-cyclam, respectively. Finally, by coupling adsorption with ultrafiltration in the tangential mode, the removal of Cu(II), Ni(II) and Zn(II) ions was found to be improved, allowing to reach a removal efficiency of 99% towards Cu(II), Ni(II) and Zn(II) ions at a metal concentration of 50 mg L −1 , and a promising removal efficiency around 70% at a very high metal concentration of 1200 mg L −1. The mechanisms involved in the capture of the metal ions by modified membranes and colloids are also discussed.