A highly dispersive nickel catalyst supported on microfiber attapulgite (MFA) was prepared. Benzene, naphthalene, triphenylmethane, 9-phenylanthracene, 1-methoxynaphthalene (MON), benzyloxybenzene, and oxybis(methylene)dibenzene were used as coal-related model compounds (CRMCs) to evaluate the catalytic activity. A conventional Ni/MFA (Ni/MFA-C) was prepared by an impregnation method. Ni/MFA is significantly active for catalytic hydroconversion of the CRMCs than Ni/MFA-C. Ni/MFA-catalyzed hydroconversions of industrial low-temperature coal tar (LTCT) and high-temperature coal tar (HTCT) were also investigated. The results show that the C-ar-O bond in MON was specifically cleaved over Ni/MFA followed by catalytic hydrogenation of the resulting naphthalene to afford tetralin. Both unsaturated hydrocarbons and heteroatom-containing organic compounds in the LTCT and HTCT were completely hydroconverted to alkanes over Ni/MFA under optimum conditions, indicating that Ni/MFA catalyzes both hydrocracking and hydrogenation. According to multiple analyses, nickel nanoparticles were formed on the surface of MFA in Ni/MFA. (C) 2014 Elsevier B.V. All rights reserved.