Geological CO₂ storage is an emerging topic in energy and environmental community, which is, as a commonly accepted sense, considered as the most promising and powerful approach to mitigate the global carbon emissions during the transition to net‐zero. Of the geological media which initially considered cover the saline aquifers, oil and gas reservoirs, coal beds, and potentially basalts, up to now only the first two choices have been proven to be the most capable storage sites and successfully implemented at pilot/commercial scales. Here, two tandem papers propose novel strategies for the first time, by synthesizing and utilizing new high‐dryness CO₂ foam, to enhance geological CO₂ storage capacity in saline aquifer and oil and gas reservoirs. In this paper, a new high‐dryness CO₂ foam is synthesized and injected into the saline aquifers to explore the storage capacity enhancement, with the unique foam‐induced advantages of sweep area expansion and storage efficiency improvement. Such a new idea is specifically evaluated and validated through a series of static analytical and dynamic performance experiments. With the optimum surfactant concentration of 0.5 wt%, the foaming volume and quality are determined to be 521 mL and 80.81%, respectively, which also shows excellent salt tolerance with 45,000 ppm Na⁺, 25,000 ppm Ca²⁺, and 25,000 ppm Mg²⁺. Moreover, the water consumption for CO₂ storage decreases from 464.31 g/mol at 25% foam quality to 67.38 g/mol at 85% foam quality by using the new CO₂ foam. Overall, the newly synthesized CO₂ foam could effectively enhance geological CO₂ storage capacity and concurrently diminish water consumption, therefore realizing the win‐win environment and economic benefits.

In this paper, effects of temperature, initial oil and injection gas compositions, and feed gas–oil ratio on oil–CO ₂ interfacial tensions, interfacial thicknesses, and minimum miscibility pressures (MMPs) in nanopores are specifically studied.