The over-consumption of fossil fuels resulted in the large quantity emission of carbon dioxide(CO2), which was the main reason for the climate change and more extreme weathers. Hence, it is extremely pressing to explore efficient and sustainable approaches for the carbon-neutral pathway of CO2 utilization and recycling. In our recent works with this context, we developed successfully a novel “chemical vapor deposition integrated process(CVD-IP)” technology to converting robustly CO2 into the value-added solid-form carbon materials.The monometallic Fe Ni0–Al2O3(FNi0) and bimetallic Fe Nix–Al2O3(FNi2, FNi4, FNi8 and FNi20) samples were synthesized and effective for this new approach. The catalyst labeled FNi8 gave the better performance, exhibited the single pass solid carbon yield of 30%. These results illustrated alternative promising cases for the CO2 capture utilization storage(CCUS), by means of the CO2 catalytic conversion into the solid-form nano carbon materials. The over-consumption of fossil fuels resulted in the large quantity emission of carbon dioxide (CO2), which was the main reason for the climate change and more extreme weathers. Hence, it is extremely pressing to explore efficient and sustainable approaches for the carbon- neutral pathway of CO2 utilization and recycling. In our recent works with this context, we developed successfully a novel “chemical vapor deposition integrated process (CVD-IP) ” technology to converting robustly into CO2 into the value-added solid-form carbon materials The catalyst labeled FNi8 gave the better performance, exhibited the single pass solid carbon yield of 30%. These results illustrated alternative promising cases for the CO2 capture utilization storage (CCUS), by means of the CO2 catalytic conversion into the solid-form nano carbon materials.