Zeolitic materials were synthesized from coal fly ash (CFA) using the fusion/hydrothermal method. The effect of NaOH/CFA ratio and particle size on the morphological structure of the zeolitic material crystals prepared was investigated by analyzing crystals morphology and crystallinity. The chemical composition, morphology, and crystallinity of the synthesized materials were characterized by SEM, XRD, and XRF. It was possible to synthesize chamfered-edged cubic crystals at NaOH/CFA ratio of 0.9. The particle size of the zeolite crystals tended to decrease with increasing the alkali content of NaOH/CFA from 0.9 to 1.8. The morphological structure of the crystalline particles was similar to that of zeolite A synthesized from the CFA. This study has shown that the fusion/hydrothermal method is a very effective technique for synthesizing the zeolitic materials from the CFA and provides a potential application for obtaining commercial products.