Acid mine drainage/lakes (AMD/AMLs) have a low pH with high concentrations of metals and sulfate and have been a major environmental problem in the Can Coal Basin, in northwestern Turkey. In this study, metal removal from Hayirtepe AML by using fly ash (FA) and modified fly ash (MFA) was investigated in batch experiments. The effects of various parameters, such as ultrasonic frequency, dose, contact time, pH, and temperature, were examined to determine the optimum conditions for metal removal from AML. This study also focused on the application of ultrasound-assisted modification by using a 20-kHz ultrasonic probe and a 40-kHz ultrasonic bath to increase the FA surface and improve its adsorption capacity for metal removal. FA modification at 20 kHz showed better results than that at 40 kHz because it produced rapid bubble implosion with acoustic cavitation. The FA and MFAs selectivity for metal removal was 98%-99% for Fe, 96%-99% for Al, 94%-97% for Zn, 90%-95% for Co, 88%-94% for Ni, 77%-92% for Cu, and 74%-92% for Mn according to the determined optimum parameters. Scanning electron microscopy coupled with the energy-dispersive X-ray spectroscopy (SEM/EDX) and X-ray diffractometry of the solid residues (SRs) identified gypsum as a new mineral phase from sulfate removal from the AML. Inductively coupled plasma mass spectrometry and SEM/EDX analysis revealed that the metal content of the SRs increased. The adsorption process fitted the pseudo-second order kinetic model. Thermodynamic parameters showed that the process was exothermic and the randomness of the solid/solution interface increased during adsorption. Reuse experiments indicated that the MFAs were reused more effectively for metal removal from AML compared with the FA. This study showed that the use of MFAs with a high adsorption capacity and surface area is economic and efficient for metal removal from AML.