In accordance with one or more embodiments of the present disclosure, a method of subsurface sequestration of CO2 in a geological basin includes identifying one or more subsurface sequestration locations in the geological basin and injecting an aqueous CO2 solution to be sequestered into the geological basin. The one or more subsurface sequestration locations are regions of deeper geological structure, relative to an adjacent shallower geological structure, into which a negatively buoyant fluid injected into the basin will sink. The aqueous CO2 solution comprises a density that is greater than the density of the water naturally present in the geological basin, such that the injected aqueous CO2 solution pools in the one or more subsurface sequestration locations.