A hydrothermal technique was employed to synthesize Ni/Mg/Al ternary L.D.H.s modified with montmorillonite (NMA-MMT-LDHs). Many characterization methods, including X-ray diffraction (XRD), scanning electron microscopy (S.E.M.), Fourier transform infrared (FTIR), and Brunauer, Emmett, and Teller (B.E.T.), were used to assess the physiochemical properties of the produced analytes. Congo red and methylene blue were utilized as model dyes to treat textile waste with the synthesized analytes. The batch adsorption model was utilized to conduct the adsorption experiments under varying contact time, adsorbent dosage, and solution pH conditions. A pseudo-second-order kinetics and the Langmuir adsorption model control the adsorption process. The maximum monolayer adsorption capacities of C.R. and M.B. were determined to be 344 and 200 mg/g, respectively. As the quantity of dosage increased from the 0.01–0.04 g, the percent removal efficiency (%) increased from 75 to 87 % for S2-LDH, 84–88 % for S2-MMT, 86–93 % for S3-MMT, and 95–97% for S4-MMT for C.R. dye and 82–85 % for S2-LDH, 83–89 % for S2-MMT, 83–91 % for S3-MMT, and 84–92 % for S4-MMT for M.B. dye. The removal percentage of C.R. dye for adsorbents S2-LDH, S2-MMT, S3-MMT, and S4-MMT were 75 %, 84 %, 86 %, and 95 %, respectively and 82 %, 83 %, 83 %, and 85 %, respectively for the M.B. dye removal. The presence of MMT significantly increases the affinity of Ni/Mg/Al-LDHs (NMA-LDHs), and the designed production technique can be used to produce a variety of compositionally distinct adsorbent materials.