Coal gangue, a solid waste produced in coal production, had caused serious environmental pollution due to accumulation on dumps. Embankment filling can solve the problem while significantly consuming the amount of coal waste for mining. The main purpose of this study is to investigate the mechanical properties and microscopic structure of coal gangue when it is subjected to erosion from water environment with different acidity. Using immersion testing to evaluate its stability in different hydro-chemical environments. Mechanical property parameters of coal gangue treated by solutions were investigated. The action microstructure of coal gangue was revealed through a series of X-ray diffraction (XRD), X-ray fluorescence spectrometry (XRF), scanning electron microscopy (SEM), and energy dispersive spectrometry (EDS). The results show that acidic solution behaved better improvement effect on compressive modulus and fraction of coal gangue samples owing to the generation of quartz and the reduction of aluminum, dissolving of some substances, and transforming of small scattered angular grains through soaking treatment. Alkalinity treatment can be chosen to improve cohesion of coal gangue as a result of polymeric silicon aluminum salt, with high viscosity, was produced by chemical reaction during immersion. Therefore, aqueous solution treatment contributes to engineering properties and presents great potential in both supplement road building materials and recycling of coal gangue.