A series of large-pore mesoporous RuNi-doped TiO2-Al2O3 nanocomposites were prepared by a facile sal-gel method using a one-pot protocol based on evaporation-induced self-assembly. Owing to high density of active sites, an open nanoarchitecture and highly promotional efficiency by synergetic effects, the as-prepared nanocomposites demonstrated excellent catalytic properties in selective CO methanation (CO-SMET). The final concentration of CO can be reduced to less than 50 ppm with more than 50% selectivity over the MRNAT-30Ni catalyst. The working temperature window covered the typical working range of 200-250 degrees C in conventional upstream low-temperature shift reactors. The MRNAT-30Ni catalyst has excellent stability during 200 h time on stream with no detectable change in CO and CH4 concentrations, and CO in outlet reaches level below 20 ppm under realistic reaction conditions. This remarkable improvement of activity/selectivity and stability could lead to wide implementation of this one-pot protocol for the synthesis of large-pore mesoporous nanocomposite catalysts for the CO-SMET process. (C) 2014 Elsevier B.V. All rights reserved.