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The development of methanation catalysts with a high catalytic activity at low temperatures and a long-term durability at high temperatures is still challenged by the conflicting constraint on the catalyst design. In this work, Ni(NO 3) 2 ·6H 2 O. and ordered mesoporous alumina (OMA) containing different amounts of the P123 template were co-ground to prepare Ni/OMA catalysts. Results indicate that NiO was embedded in the meso-channels of OMA via the solid-state grinding. Moreover, the metal particle size, dispersion and reducibility of the catalyst can be easily regulated by the amount of the residual P123 template in OMA, which can be simply controlled by changing the treatment temperature of the OMA precursor. The optimized 15Ni/OMA-120 with a high dispersion and small size of metallic Ni showed high low-temperature catalytic activity with TOF of 31.5 h−1 and STY of 319.1 mol CH4 g cat h−1 at 340 °C, but also demonstrated good anti-sintering and coke-resistance performance with a time-on-stream of 150 h long-term durability at 600 °C, which is comparable with the counterpart 15Ni-OMA prepared by traditional wet-process of one-pot evaporation induced self-assembly. [Display omitted] • High-performance Ni/OMA catalyst was prepared by solid-state grinding method. • The interaction between residual template and Ni precursor could be regulated. • Ni/OMA catalyst showed high dispersion and small size of metallic Ni. • 15Ni/OMA-120 showed both a high activity and good stability at high temperatures. [ABSTRACT FROM AUTHOR]