Mechanically treated fly ash (FA) was utilised to provide Al and Si atoms for zeolite synthesis. A combination of mechanical fly ash activation and classical hydrothermal synthesis led to favourable dissolution of activated fly ash and improved crystallization of zeolites. The milling activation step induced structural changes in FA to promote its reactivity in alkaline solution. The conversion of milled FA into zeolite materials was finally completed in the second step, during hydrothermal synthesis. The effect of such factors as crystallization temperature, milling time, and solution conditioning were systematically studied. The physicochemical properties characterising the obtained zeolite materials were determined via particle size distribution (PSD), nitrogen adsorption–desorption, X-ray fluorescence spectroscopy (XRF), scanning electron microscopy (SEM), and powder X-ray diffraction (XRD). As a result, the best samples achieved a high degree of crystallinity and an extensive specific surface area of 292 m2/g, 87.4 m2/g, 41.9 m2/g for Na-X, Na-P1, and Na-A, respectively. The obtained results provide new and useful data for utilising fly ash resources and synthesising other practical zeolites through an innovative, mechanochemically assisted, and template-free approach.