In order to find an efficient and economical wetland substrate to treat mine wastewater containing various heavy metals, and effectively realize the resource utilization of water treatment residuals, in this paper, the treatment efficiency of mine wastewater containing various heavy metals was investigated using unburned ceramsite prepared from water treatment residuals (UCWTR) and clay ceramsite. The continuous dynamic test results showed that the removal rate of Pb, Cd, Cu, Zn, and Fe can reach more than 98.5% after the UCWTR-based CWs runs for 56 days, and its concentration was 30.05%, 24.85%, 20.82%, 14.63%, and 7.91% lower than that of the clay ceramsite-based CWs, respectively. SEM, XPS, and FT-IR showed that the characteristic peaks of two ceramsites were basically similar. The ceramsite undergoes ion exchange, coordination complexation, and chelation reaction with Pb, Cd, Cu, Zn, and Fe under the action of the gel of internal groups -OH, C=O, Al-OH, Si-Fe-O and C-S-H. Compared with clay ceramsite, the ion exchange reaction and chelation reaction of -OH effect and the coordination reaction of C=O effect of carboxyl group in UCWTR were enhanced. In conclusion, using UCWTR as a CWs substrate can effectively enhance the adsorption capacity of heavy metals, providing a scientific basis for the application of UCWTR-based CWs in mine wastewater treatment.