Developing highly active hydrodesulfurization (HDS) catalysts is very important for ultraclean fuel production. Here, we report the successful preparation of crystalline mordenite nanosheet assemblies (NS-HMOR) with large external surface area and micro-mesoporous structure. After introduction of nickel and phosphorus species into NS-HMOR and its activation, the obtained Ni2P/NS-HMOR catalyst exhibits higher HDS activity (TOF = 1.9 x 10(-3) s(-1)) and better stability in 4,6-dimethyldibenzothiophene HDS than a silica-supported Ni2P catalyst (TOF = 1.3 x 10(-3) s(-1)). The large number of acidic hydroxyl groups on the NS-HMOR surface facilitates the formation of very small Ni2P clusters on the outer surface, and the open micropores at the NS-HMOR surface help to prevent their aggregation. (C) 2016 Elsevier Inc. All rights reserved.