CO2 capture is an enabling technology for carbon conversion and storage; however, the high costs of the process have hindered its large‐scale application so far. Therefore, new approaches for carbon abatement, particularly from diluted sources, are urgently needed. Herein, based on the adsorption and catalysis bifunctionality of 2D‐layered Ni–O–Al2O3 nanosheets, a two‐step “capture and methanation” process is reported for the removal and utilization of CO2, with no additional energy input for desorption being required. Continuous and nearly 100 % capture of CO2 was demonstrated at low temperatures (≤250 °C) and prolonged cycles. At isothermal conditions, the material could be fully regenerated with the production of methane, showing considerably higher time efficiency than temperature‐swing and pressure‐swing technologies. This strategy may pave a new way for CO2 reduction, providing a scalable connection between the power grid and the gas grid when H2 is used.