In this study, cetyltrimethylammonium bromide-modified multi-layered Ti3C2Tx MXene (CMM) was produced using a Ti3AlC2 precursor, and its capacity to remove the anionic dye, methyl orange (MO), was investigated in detail. An electrostatic combination between negatively charged Ti3C2Tx nanosheets and cationic surfactant solution (CTAB) produced this adsorbent. This triggered an exposure of the accessible active sites to further boost adsorption effectiveness by increasing the distance between the MXene nanosheets. Prepared adsorbents were characterized using some analytical techniques, including TGA, FESEM, EDX, FTIR, XRD, and N2 adsorption-desorption. Furthermore, some influencing parameters such as contact time, solution of pH, loading adsorbent, and initial dye concentration were evaluated, with findings showing that MO could adsorb CMM to its maximum capacity at an adsorbent dosage of 0.83 g/L, a contact time of 90 min, and a solution pH of 3. Adsorption results were found to be highly linked with both Langmuir isotherm (R2 = 0.9990) and the pseudo-second-order kinetic model (R2 = 0.9924). The maximum adsorption capacity of MO was obtained at approximately 213.00 mg/g. Also, hydrogen bonding, π-cation interactions, and electrostatic adsorption can all be implicated in the mechanism of MO adsorption on CMM. The fabricated CMM is presented as a prospective adsorbent for the removal of dyes from polluted water, demonstrating robust recyclability for up to the fifth iteration. All these outstanding properties indicate that cetyltrimethylammonium bromide-modified multi-layered Ti3C2Tx MXene can be considered as applicable adsorbents for textile pollutants.