This article proposes a novel sodium dodecylbenzenesulfonate (SDBS)-assisted equilibrium adsorption method for preparing highly dispersed Ni/Al2O3 and Fe -promoted NiFe/Al2O3 thioetherification catalysts. The proposed strategy anchors nickel cations onto the electronegative surface of an Al2O3 support modified by negatively charged DBS- bilayers. As a result, this method achieves highly dispersed Ni nanoparticles without strengthening the metal-support interaction, promoting the reducibility and sulfurization of the supported Ni species. The as-prepared Ni-based catalysts have a smaller size, a higher dispersion of metal nanoparticles, and a greater amount of active metal sulfides than their counterparts prepared by the conventional impregnation method, endowing them with excellent catalytic performance for the highly selective removal of mercaptans. This method provides a new opportunity to prepare highly dispersed metal nanoparticles without a strong metal support interaction.