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Abstract One of the critical factors that control the efficiency of CO 2 geological storage process in aquifers and hydrocarbon reservoirs is the capillary‐sealing potential of the caprock. This potential can be expressed in terms of the maximum reservoir overpressure that the brine‐saturated caprock can sustain, i.e. of the CO 2 capillary entry pressure. It is controlled by the brine/CO 2 interfacial tension, the water‐wettability of caprock minerals, and the pore size distribution within the caprock. By means of contact angle measurements, experimental evidence was obtained showing that the water‐wettability of mica and quartz is altered in the presence of CO 2 under pressures typical of geological storage conditions. The alteration is more pronounced in the case of mica. Both minerals are representative of shaly caprocks and are strongly water‐wet in the presence of hydrocarbons. A careful analysis of the available literature data on breakthrough pressure measurements in caprock samples confirms the existence of a wettability alteration by dense CO 2 , both in shaly and in evaporitic caprocks. The consequences of this effect on the maximum CO 2 storage pressure and on CO 2 storage capacity in the underground reservoir are discussed. For hydrocarbon reservoirs that were initially close to capillary leakage, the maximum allowable CO 2 storage pressure is only a fraction of the initial reservoir pressure.