Water pollution by hexavalent chromium, Cr(VI), poses serious concerns due to its detrimental public health effects. In this work, we report the synthesis, characterization, and sorption properties for Cr(VI) by MoS₄^2- intercalated layered double hydroxide, CoAl-MoS₄-LDH (CoAl-MoS₄). Our results show that CoAl-MoS₄ can effectively remove Cr(VI) ions from acidic, neutral, and basic media. At neutral medium, it exhibits a very strong affinity, K_d ∼ 1.91 × 10⁵ mL/g, toward Cr(VI) ions. Under such conditions, this material can remove over 99% of Cr(VI) from a ∼10⁴ ppb of Cr(VI) contaminated solutions, leaving behind residual concentration below the World Health Organization (WHO) defined limit for drinking water. Moreover, our study shows that CoAl-MoS₄ is a highly-competent Cr(VI) adsorbent exhibiting a removal capacity (q_m) as high as ∼231 mg/g. The CoAl-MoS₄ follows pseudo-second order rate kinetics for the sorption of chromate, and the concentration dependent sorption data can be fitted well with the Langmuir sorption isotherm. Furthermore, CoAl-MoS₄ is highly selective to Cr(VI) ions in the presence of various competitive ions in contaminated water systems. All these results suggest that CoAl-MoS₄ is a very efficient sorbent for decontamination of hexavalent chromate from wastewater systems. Graphical Abstract