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CO/CO2 hydrogenation has attracted much attention as a pathway to achieve carbon neutrality and production of synthetic natural gas (SNG). In this work, two-dimensional NiAl layered double oxide (2D NiAl-LDO) has been successfully decorated by SiO2 nanoparticles derived from SiCl4 and used as CO/CO2 methanation catalysts. The as-obtained H-SiO2-NiAl-LDO exhibited a large specific surface area of 201 m2/g as well as high ratio of metallic Ni0 species and surface adsorption oxygen that were beneficial for low-temperature methanation of CO/CO2. The conversion of CO methanation was 99% at 400 °C, and that of CO2 was 90% at 350 °C. At 250 °C, the CO methanation reached 85% whereas that of CO2 reached 23% at 200 °C. We believe that this provides a simple method to improve the methanation performance of CO and CO2 and a strategy for the modification of other similar catalysts.