In the recent decade, injection of nanoparticles (NPs) into underground formation as liquid nanodispersions has been suggested as a smart alternative for conventional methods in tertiary oil recovery projects from mature oil reservoirs. Such reservoirs, however, are strong candidates for carbon geo-sequestration (CGS) projects, and the presence of nanoparticles (NPs) after nanofluid-flooding can add more complexity to carbon geo-storage projects. Despite studies investigating CO2 injection and nanofluid-flooding for EOR projects, no information was reported about the potential synergistic effects of CO2 and NPs on enhanced oil recovery (EOR) and CGS concerning the interfacial tension (γ) of CO2-oil system. This study thus extensively investigates the effect of silica NPs on the γ of CO2/decane system at elevated pressure and temperature to recognise the potential impact of NPs-injection on the future CGS projects. To achieve this, a wide-ranging series of tests have been conducted to reveal the role of hydrophilic and hydrophobic silica NPs on γ of the CO2/oil system. n-decane was utilized as model oil and different amounts of NPs were mixed with the oil phase. Oil-NPs dispersions were formulated using an ultrasonic homogenizer. The γ of the CO2/oil system was measured at different pressures (0.1 to 20 MPa) and temperatures (25 to 70 °C) using a high-pressure temperature optical cell. The γ data were measured using the pendant drop technique via axisymmetric drop shape analysis (ADSA). The results showed that, generally, CO2/oil γ subjected mainly to pressure, temperature, and with less extent to NPs load in the oil phase. γ decreases with increased pressure until reaching a plateau where no more significant decrease in γ was observed. The γ trend with increased temperature, on the other hand, was more completed. No significant impact of temperature on γ was recorded with low pressure (≤ 5 MPa). Similarly, at relatively high pressure (≥ 25 MPa), only a slight variation of IFT with temperature change was recorded. However, for the pressure range from 5 – 25 MPa, IFT was increased remarkably with temperature. Furthermore, NPs in the oil phase exhibit a remarkable influence on IFT. In this context, the presence of hydrophilic silica NPs in the oil phase can significantly reduce the γ of the CO2/decane system. However, hydrophobic silica NPs showed less influence on IFT reduction. The outcomes of this work afford good understandings into applications of NP for EOR and CGS applications and help to de-risk CO2-geological storage projects.