Ever-increasing CO2 emissions and atmospheric concentration mainly due to the burning of traditional fossil fuels have caused severe global warming and climate change problems. Inspired by nature’s carbon cycle, we propose a novel dual functional catalyst-sorbent to tackle energy and environmental problems simultaneously via direct capture of CO2 from air and in-situ solar-driven conversion into clean fuels. Economically and operationally advantageous, the planned coupling reaction can be carried out in a single reactor without the requirement for an extra trapping device. The great CO2 capture and conversion performance in an integrated step is shown by the CO2 capacity of up to 0.38 mmol·g−1 for adsorption from 500 ppm CO2 at 25 °C and the CO2 conversion rate of up to 95%. Importantly, the catalyst-sorbent is constituted of a nonprecious metal Ni catalyst and an inexpensive commercially available CO2 sorbent, viz, zeolite NaA. Furthermore, this designed dual functional material also exhibits outstanding stability performance. This work offers a novel pathway of capturing CO2 in the air at room temperature and converting it by CH4 into fuel, contributing to the new era of carbon neutrality.