Storing excess CO2 in underground saline aquifers is an important technology for the low carbon future. Direct dissolution of CO2 molecules in connate brine (solubility trapping) is a promising carbon geosequestration method, yet the molecular-level understanding was underexplored compared to other macroscopic CO2 trapping mechanisms. Here, we show that injecting supercritical CO2 (scCO2) nanobubbles into saline aquifers can considerably boost solubility trapping. Molecular modeling predicts 1.5 to 2× CO2 oversaturation in brine with the presence of scCO2 nanobubbles for enhanced CO2 storage capacity. Furthermore, the nanobubble electrical double layers (EDL) are enhanced by reducing nanobubble sizes and increasing brine salinity, indicating enhanced nanobubble stability against CO2 macro-phase separation in saline aquifers. The unique physiochemical properties of nanobubbles, including high specific scCO2/brine interface areas and low buoyancy forces, also greatly favor the solubility trapping processes. This study highlights that combining nanobubble technology in CO2 geosequestration is a promising new direction.