The modification of silica microparticles surface with a high number of amino/carboxylic groups of polymer chains represent an interesting route to obtain nanostructured composite materials aiming different applications. Herein, four weak polycations (PC) [polyethyleneimine (PEI), polylysine (PLL), polyvinylamine (PVAm), polyallylamine hydrochloride (PAH)] and one weak polyanion [polyacrylic acid (PAA)] were layer-by-layer deposited onto spherical silica to form composite microparticles. A strategy where each deposited polycation layer was chemically cross-linked with glutaraldehyde (GA) prior to the deposition of PAA layer was used, forming at the end silica//(PCsingle bondGA/PAA)_n composite microparticles. Finally, we investigated the particles towards their adsorption properties on metal ions (Cu²⁺, Pb²⁺, Ni²⁺, and Fe²⁺) from simulated and real surface water, as a potential application for the composite particles.