Environment-friendly disposal of coal fly ash (CFA) is essential for sustainable development and cleaner production of electricity in thermal power plants. Although CFA has been employed for soil amelioration, direct application of CFA to soil may pose risks such as heavy metal contamination. This study investigated recycling of CFA through a novel method, which employs the ultrasonic treatment of CFA before its application. Physico-chemical properties of refuse dump soil and CFA were analysed. Subsequently, the effect of ultrasonic treatment on the physico-chemical properties of CFA was investigated. Different ultrasonic parameters (ultrasonic frequency, time interval, and temperature) were studied using response surface methodology. Finally, plant growth experiments were conducted to verify the feasibility of using ultrasonically treated CFA (UTCFA) for soil amelioration. The results show that untreated CFA cannot be used for soil amelioration due to its unsuitable high pH (10.20) and threatening concentrations of trace elements (6.80 mg/kg for Cadmium and 109.75 mg/kg for Arsenic). Ultrasonic treatment increases the soil amelioration properties of CFA by decreasing pH (to 8.50–9.20), decreasing concentrations of Cadmium and Arsenic (satisfying GB 15618-2018), and improving the water-holding capacity of CFA (reducing water loss). Plant indicators confirm the feasibility of using UTCFA for soil amelioration and suggest that the optimum UTCFA proportion is 20%. This study is a benchmark for the utilisation of ultrasonic treatment to improve the soil amelioration properties of CFA.