Abstract Nanofluids are proven to be efficient agents for wettability alteration in subsurface applications including enhanced oil recovery (EOR). Nanofluids can also be used for CO 2 -storage applications where the CO 2 -wet rocks can be rendered strongly water-wet, however no attention has been given to this aspect in the past. Thus in this work we presents contact angle (θ) measurements for CO 2 /brine/calcite system as function of pressure (0.1 MPa, 5 MPa, 10 MPa, 15 MPa, and 20 MPa), temperature (23 °C, 50 °C and 70 °C), and salinity (0, 5, 10, 15, and 20% NaCl) before and after nano-treatment to address the wettability alteration efficiency. Moreover, the effect of treatment pressure and temperature, treatment fluid concentration (SiO 2 wt%) and the period of nano-treatment on the wettability of calcite is examined. We find that nano-treatment alters the wettability significantly i.e. intermediate-wet calcite turns strongly water-wet after treatment (e.g. at 20 MPa and 50 °C, θ = 64° for intermediate-wet calcite, and θ = 28° for nano-treated calcite). Consequently, pre-injection of nanofluids will significantly enhanced the storage potential. It was also found that the permanent shift in wettability after nano-treatment is a function of treatment conditions including temperature, pressure, and treatment duration time and that surfaces treated under high pressure and low temperature yield better wettability alteration efficiency. We point out that the change in wettability is attributed to the changes in surface properties of the nano-treated sample. The results of the study thus depict that nanoparticles can significantly enhance storage potential and de-risk storage projects.