In this paper, a novel catalyst support with trimodal pore structure was hydrothermally synthesized by building up nano-particles of titanium silicalite-1 inside the macroporous system of silica gel using the tetrapropylammonium hydroxide (TPAOH) as template, titanium (IV) tetrabutoxide monomer (TBOT) as titanium source and the silica gel with macropores as in situ silicon source as well as matrices. The prepared support exhibited intrinsic pore of TS-1, intercrystalline mesopores and residual macropores of silica gel. When loaded with Co, the trimodal catalyst was employed to catalyze the methanation of carbon monoxide, showing higher CO conversion and CH(4) selectivity than the bimodal and unimodal catalysts due to the favored metallic Co surface area and dispersion. (C) 2011 Elsevier B.V. All rights reserved.