A basic urea technique was successfully used to synthesize Mg/Al-Layered double hydroxides (Mg/Al LDHs), which were then calcined at 400 °C to form Mg/Al-Layered double oxides (Mg/Al LDOs). To reconstruct LDHs, Mg/Al LDOs were fabricated with different feeding ratios of Ni by the co-precipitation method. After synthesis, the Ni/Mg/Al-layered double hydroxides (NMA-LDHs) with 20% and 30% Ni (S1 and S2) were roasted at 400 °C and transformed into corresponding Ni/Mg/Al-layered double oxides (NMA-LDOs) (S1a and S2b, respectively). The physiochemical properties of synthesized samples were also evaluated by various characterization techniques, such as X-ray diffraction (XRD), Scanning electron microscopy (SEM), Energy dispersive X-ray spectroscopy (EDS), Fourier transform infrared (FTIR), and Brunauer, Emmett, and Teller (BET). The adsorption behavior of methyl orange (MO) onto the synthesized samples was evaluated in batch adsorption mode under varying conditions of contact time, adsorbent quantity, and solution pH. As the dosage amount increased from 0.01–0.04 g, the removal percentage of MO dye also increased from 83% to 90% for S1, 84% to 92% for S1a, 77% to 87% for S2, and 93% to 98% for S2b, respectively. For all of the samples, the adsorption kinetics were well described by the pseudo-second-order kinetic model. The equilibrium adsorption data were well fitted to both Langmuir and Freundlich models for methyl orange (MO). Finally, three adsorption-desorption cycles show that NMA-LDHs and NMA-LDOs have greater adsorption and reusability performance for MO dye, signifying that the design and fabrication strategy can facilitate the application of the natural hydrotalcite material in water remediation.