Hydrotalcite materials are generally utilized for anionic pollutants due to its interlayered anion exchange ability. Their potentiality for cationic contaminants is rarely explored. In this study, disulfide (S) intercalated LDH material demonstrated capability to remove both heavy metal cations and oxyanions simultaneously from water. The S intercalation of LDH significantly improved its adsorption capability towards both heavy metal cations (Co and Ni) and oxyanion (CrO). The adsorption amount of S-LDH towards Co and Ni reached 88.6mg/g and 76.2mg/g, which are 405% and 281% higher than that of pristine LDH. For CrO removal, the adsorption amount reached 34.7mg/g, 402% higher than that of pristine LDH. The cations capture mechanism mainly depends on the novel layer sheet cation substitution mechanism based on irreversible precipitation and the generation of metal sulfide precipitates. Meanwhile, the interlayered S can be easily replaced by CrO to realize the simultaneous removal of both heavy metal cations and oxyanions. In the fixed-bed column experiments, 448 bed volume (BV) (672 mL) of simulating electroplating wastewater can be efficiently treated by yielding only 1 BV(15 mL) of chemical sludge, which is practically acceptable. This work provided a highly practical adsorption technology based on the S modification hydrotalcite material for the purification of heavy metal ions contaminated wastewater.