CO2 geo-sequestration (CGS) is crucial in tackling global climate change, and the safety of CO2 storage within the reservoir is intricately linked to wettability. The utilization of nanofluids-surfactants for adjusting reservoirs’ wettability has emerged as a promising approach to enhance the security of CGS. However, the mechanism underlying their impact on reservoir wettability and carbon sequestration remains elusive. Regarding nanoactive fluid (ASNF) compounded with nano-SiO2 and AOS, to explore its potential for wettability reversal of CO2-exposed shale under in situ conditions, comparative experiments were conducted with Longmaxi Formation shale as the subject. The chemical structures and microstructures of shale before and after the experiments were comprehensively characterized. The results showed that a maximum of 67.93 % enhanced the water wettability of samples co-treated with ASNF and ScCO2. The primary reason for shale wettability reversal was increased hydrophilic chemical groups and enhanced interaction energy between organic matter and water molecules, stemming from nanoactive particle retention on the shale surface. The alteration in wettability decreased the mobility of CO2 and increased the distribution of surface water films, enhancing the carbon sequestration capabilities of the trapping mechanism. These findings provided an important foundation for improving the effectiveness and safety of CGS in shale reservoirs.