The enormous increase of heavy metal pollution has led to a rise in demand for synthesizing efficient and stable adsorbents for its treatment. Therefore, we have designed a novel adsorbent by introducing (MoS₄)²⁻ moieties within the layers of NiFeTi LDH-NO₃, via an ion exchange mechanism, as a stable and efficient adsorbent to deal with the increasing water pollution due to heavy metals. Characterization techniques such as XRD, FTIR, TGA, SEM, TEM, and Raman spectroscopy were used to confirm the formation of (MoS₄)²⁻ intercalated NiFeTi LDH and structural changes after the adsorption process. The efficiency of the material was tested with six heavy metal ions, among which it was found to be effective for toxic Pb²⁺ and Ag⁺ ions. When selectivity was studied with all six of the metal ions copresent in one solution, the material showed greater selectivity for Pb²⁺ and Ag⁺ ions with the selectivity order of Ni²⁺ < Cu²⁺ < Zn²⁺ < Fe³⁺ < Pb²⁺ < Ag⁺, with great adsorption capacities of 653 mg g⁻¹ for Pb²⁺ and 856 mg g⁻¹ for Ag⁺ metal ions. Further, the kinetics adsorption study for both the metal ions had a great correlation with the pseudo-second-order model and supported the chemisorption process via the formation of M–S bonding. The adsorption process obeyed the Langmuir model. Therefore, the MoS₄-LDH material could be a promising adsorbent for the removal of heavy metals.