The present study aimed to use geopolymer materials synthesized from different fly ashes, which are promising for the adsorption of copper ions from aqueous solutions. The characterization of fly ashes and prepared adsorbents was performed by energy-dispersive X-ray spectroscopy (EDS) analysis, Brunauer–Emmett–Teller (BET) surface area analysis, and Scanning Electron Microscopy (SEM). Taguchi and ANOVA methods were used to predict the effect of different working parameters on copper ion removal by prepared geopolymers. Based on data obtained by the Taguchi method, it was found that the factor most influencing the adsorption process is the type of adsorbent used, followed by the solution pH, the reaction time, the adsorbent dose, and the initial copper ion concentration. The ANOVA results agree with the Taguchi method. The optimal conditions of the adsorption process were: fly ash C modified by direct activation with 2 M NaOH, at 70 °C for 4 h, solution pH of 5, initial pollutant concentration of 300 mg/L, 40 g/L adsorbent dose, and 120 min of reaction time. Copper ion removal efficiency was determined experimentally under optimal conditions, achieving a value of 99.71%.