Using zeolites as catalysts of coal pyrolysis for production of valuable chemical compounds such as aromatics is being widely investigated and has shown promising results. In this study, pure faujasite-type Y zeolite crystals were successfully synthesized by a direct hydrothermal method with sodium silicate solution and colloidal silica as the silicon sources, without any seeding gel. A novel approach was adopted to directly synthesize zeolites impregnated with nickel oxide. Moreover, a batch reactor was designed to increase the silica/alumina ratio (SAR) of the zeolites by dealumination process without causing significant damage to the zeolite structure. The various analysis methods were employed to characterize the parent and modified zeolites, and the fabricated zeolites were applied in coal pyrolysis experiments. The results are presented in order to show the catalytic performance of the faujasite-type Y zeolites for application in coal pyrolysis process.