The adsorption of Congo red from solution was carried out using calcium-rich fly ash with different contact times, concentrations, temperatures, and pHs. While the amount of dye adsorbed per unit weight of fly ash increases with increasing concentration and temperature, it decreases slightly with increasing pH. The adsorption was between 93 and 98% under the conditions studied. Kinetic studies showed that the adsorption process obeyed the pseudo-second-order kinetic model. It was also determined that the adsorption isotherm followed Freundlich and Dubinin-Radushkevich models. From thermodynamic studies, it was seen that the adsorption was spontaneous and endothermic. Desorption studies suggested that desorption was 29.18% in the presence of 0.1 N HCl and was 47.21% in the presence of CH(3)COOH (50% v/v). This indicated that most of the dye was held by fly ash via chemisorption as well as ion exchange. Furthermore, FTIR study also shows that a chemisorption process occurs between CR and fly ash, probably indicating dye/fly ash complexing.