During clarification processes of raw water, a vast amount of by‐product known as “drinking water‐treatment residuals” (WTRs) are produced, being principally composed of hydroxides of the Al or Fe salts added during water treatment plus the impurities they remove. Aluminum‐based (Al‐WTR) and iron‐based (Fe‐WTR) materials were applied at 10% w/w to degraded, bare (unvegetated) soils from a restored coal mining site in central England (pH <3.9) to study their potential amelioration effects on earthworm mortality, biomass yield of seedling plants, and element concentrations in plant tissues, earthworm tissues, and soil solutions. A separate treatment with agricultural lime was also conducted for comparison to evaluate whether any observed improvements were attributable to the liming capacity of the WTRs. After completion of the trials, all samples were subjected to a wet–dry cycle, and the experiments were repeated (i.e., simulating longer‐term effects in the field). Both types of WTRs significantly increased the biomass of plants, and in some treatments, survival of earthworms was also enhanced compared to nonamended soils. Excess plant tissue element concentrations and element concentrations in soil solutions were reduced in amended soils. The implications are that adding WTRs to mining‐impacted soils is a potentially viable, sustainable, and low‐cost remediation method that could be used globally to improve the soil condition. Environ Toxicol Chem 2020;39:1277–1291. © 2020 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals, Inc. on behalf of SETAC.