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This investigation reveals the adsorption characteristics of two basic dyes, thionine (TH) and safranine T (ST), onto fly ash (FA) and its three zeolitized products prepared at different hydrothermal conditions. Typical two-step isotherms were observed for TH adsorption onto four adsorbents, whereas the isotherms of the larger ST molecules were S-shaped. The adsorption capacities of the zeolitized fly ash (ZFA) estimated from the first plateau region of the TH isotherms was nearly twice the FA capacity. The capacities increased by up to five times in the second plateau region. The adsorption capacity of FA for ST is equivalent that of TH, whereas the capacities of ZFA are lower than those found for TH. The equilibrium results were well-described by the Freundlich isotherm model. The kinetic data obtained in the temperature range of 298–318 K was analyzed using Paterson's and Nernst Plank's approximations based on the homogeneous surface diffusion model (HSDM). The thermodynamic functions for the transition state were evaluated from the temperature-dependence of the surface diffusion coefficients by applying the Eyring model.