This article proposes a novel gemini surfactant-assisted synthesis of Mo precursor for preparing NiMo/SiO2-Al2O3 ultra-deep hydrodesulfurization (HDS) catalysts. The proposed method transforms polymolybdate anions into gemini surfactant-linked Mo precursor (GSMP), which facilitates the formation of highly dispersed MoS2 phases with improved stacking and therefore produces a large number of accessible Ni-Mo-S phases after Ni incorporation. The GSMP-based NiMo/SiOa-Al2O3 catalyst presents higher catalytic activity for the HDS of 4,6-dimethyldibenzothiophene and fluid catalytic cracking (FCC) diesel than its counterparts prepared via impregnation and the cetyltrimethylammonium bromide assisted hydrothermal method. (C) 2016 Elsevier B.V. All rights reserved.