Previous studies in our laboratory have demonstrated that drinking-water treatment residuals are effective sorbents of arsenic V. However, the effect of soil solution chemistry on arsenic V sorption by drinking-water treatment residuals-amended soils remains to be explored. The current study uses a batch incubation experimental set up to evaluate the effect of soil solution pH, competing ligands, and complexing metal on arsenic V sorption by a sandy soil (Immokalee series) amended with two rates (25 and 50 g kg−1) of aluminum and iron-based drinking-water treatment residuals. Experiments were conducted at three initial arsenic loads (125, 1,875, 3,750 mg kg−1) and a constant solid: solution ratio of 200 g L−1. An optimum equilibration time of 8 days, obtained from kinetic studies, was utilized for sorption experiments with both aluminum and iron drinking-water treatment residual-amended soil. Presence of phosphate decreased arsenic V sorption by both aluminum and iron drinking-water treatment residual amended soils, with a strong dependence on pH, drinking-water treatment residual types, drinking-water treatment residual application rates, and phosphate concentrations. Addition of sulfate had no effect on arsenic V sorption by aluminum or iron drinking-water treatment residual-amended soil. A complementing effect of calcium on arsenic V sorption was observed at higher pH. Results elucidating the effect of soil solution chemistry on the arsenic V sorption will be helpful in calibrating drinking-water treatment residual as a sorbent for remediation of arsenic-contaminated soils.