Coal fly ash-derived zeolites have attracted considerable interest in the last decade due to their use in several environmental applications such as the removal of dyes and heavy metals from aqueous solutions. In this work, coal fly ash-derived zeolites and silver nanoparticles-impregnated zeolites (nanocomposites) were synthesized and characterized by TEM/EDX, SEM/EDX, XRD, XRF, porosimetry (BET), particle size analysis (PSA) and zeta potential measurements. The synthesized materials were used for the removal of Hg2+ from aqueous solutions. The results demonstrated that nanocomposites can remove 99% of Hg2+, up to 10% and 90% higher than the removal achieved by the zeolite and the parent fly ash, respectively. Leaching studies further demonstrated the superiority of the nanocomposite over the parent materials. The Hg2+ removal mechanism is complex, involving adsorption, surface precipitation and amalgamation.