Deep desulfurization by pi-complexation is an efficient technique for purification of fuels. In pi-complexation adsorbents, Cu(I)-based materials are effective due to low cost and high activity. However, the deep desulfurization has been proven to strongly rely on the dispersion extent of Cu species. Herein, for the first time, we report ammonia assisted deposition precipitation one-step N-2 reduction strategy to fabricate Cu2O-containing KIT-6. In such strategy, Cu(NO3)(2) precursor was directly introduced into the microenvironment exist between template and silica walls of template-P123-containing KIT-6 via ammonia assisted deposition precipitation. The subsequent single step N-2 reduction strategy perform three functions in a single mode i.e. decomposition of Cu precursor to CuO, template removal, and conversion of CuO to Cu(I). Our strategy is convenient and efficiently promoted the dispersion of Cu species with high yield (61.84%) of Cu(I). We also demonstrated that the resultant material, as-synthesized KIT-6 supported with an optimal content 20 wt% of Cu, can capture 0.28 mmol.g(-1) thiophene, which is obviously better than its counterpart CuCK-20 synthesized via calcined KIT-6. Furthermore, the thiophene adsorption activity can be recovered well without any obvious loss. Facile synthesis, high thiophene removal, and excellent regeneration ability make Cu/KIT-6 favorable for utilization in adsorptive desulfurization technology.