This study investigated a low-energy-consuming procedure for the synthesis of zeolite materials from coal fly ash (CFA). Materials containing zeolite phases, namely Na–X, Na–P1, and zeolite A, were produced from F–class fly ash, using NaOH dissolved in distilled water or in wastewater obtained from the wet flue gas desulphurization process, under atmospheric pressure at a temperature below 70 °C. The influence of temperature, exposure time, and alkaline solution concentration on the synthesized materials was tested. In addition, chemical, mineralogical, and textural properties of the obtained materials were determined by X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy (SEM), and cation exchange capacity (CEC). Cd(II), Ni(II), NH4+ cation, and Se(VI) anion sorption experiments were conducted to compare the sorption properties of the produced synthetic zeolites with those of the commercially available ones. Zeolitization resulted in an increase of CEC (up to 30 meq/100 g) compared to raw CFA and enhanced the ability of the material to adsorb the chosen ions. The obtained synthetic zeolites showed comparable or greater sorption properties than natural clinoptilolite and synthetic Na–P1. They were also capable of simultaneously removing cationic and anionic compounds. The structural, morphological, and textural properties of the final product indicated that it could potentially be used as an adsorbent for various types of environmental pollutants.