Over the past few years, population growth, industrial progress and climate change have led to water scarcity. Thus, water pollution caused by hazardous soluble and insoluble pollutants, such as toxic metals and phenolic compounds, has become an important problem that should be dealt with urgently. For instance, new methods have been introduced to convert low-cost raw materials (i.e. coal fly ash and coal bottom ash "wastes-to-resource") into suitable materials for new cleaner production to achieve sustainability goals in wastewater-containing toxic metals and phenolic compounds purification. Obviously, the functionalization of coal fly ash and bottom ash enhances the ability of coal ash-based entities as potential materials in wastewater remediation technologies. Here, we review the application of coal ashes, including coal bottom ash and fly ash-based materials for toxic metals and phenolic compounds removal. We also examine their structural properties and functionalization to enhance their affinities toward these pollutants in aqueous environment. Even though each process has its own benefits and limitations, coal ash-based materials appear promising for the removal of toxic metals and phenolic compounds using adsorption, membrane filtration, and photocatalysis. Overall, the study on the availability of coal fly ash and bottom ash for wastewater treatment have resulted in high removal efficiencies for toxic metals and phenolic compounds. In the future, new recycling methods for coal ashes as new water purification agents should be further studied and advanced processes should be investigated in order to achieve wastewater remediation purposes.