A highly active and sulfur-tolerant 3 wt% Pd2Si/CNTs catalyst was prepared by chemical vapor deposition, in which dichlorodimethylsilane was used as an Si source. The as-prepared catalyst was used as an efficient catalyst for deep hydrodesulfurization (HDS) of dibenzothiophene and 4, 6-dimethyldibenzothiophene. The HDS activity over 3 wt% Pd2Si/CNTs is three times higher than that of the commercial NiMoS/Al2O3 catalyst and significantly higher than that of the other traditional metal silicide catalysts. In addition, this Si-modified catalyst shows a preference for the direct desulfurization (DDS) pathway for HDS and excellent stability in the 80 h HDS life test. (C) 2018 Elsevier Inc. All rights reserved.