Supercritical carbon dioxide (SCCO2) fracturing fluid is an excellent application in CO2 re-use. It has many advantages than water-based fracturing fluids. However, the low viscosity hinders its application in unconventional oil and gas reservoirs. Therefore, we tried to improve the property of SCCO2 fracturing fluid by increasing the viscosity. A thickened SCCO2 fracturing fluid was constructed and the fracturing property of the fracturing fluid was investigated. The fracturing fluid consisted of toluene (cosolvent), polydimethyl silicone (thickener) and SCCO2. In SCCO2, toluene and polydimethyl silicone obtain low miscible pressure at 42 °C. In addition, the constructed fracturing fluid system obtains higher viscosity value (as high as 1.5 mPa·s), which can be 40 times high than the viscosity of pure SCCO2 at 42 °C and 20 MPa. These features match the viscosity requirement as a fracturing fluid. Molecular dynamics (MD) simulations were carried out to study the solubility parameter of the fracturing fluid system in molecular level. These MD simulation results show that, as a cosolvent, toluene helps polydimethyl silicon dissolve in SCCO2, which is consistent with laboratory experiment results. Moreover, the studied fracturing fluid obtains good properties as a fracturing fluid in terms of high proppant carrying capability, low fluid leakoff coefficient, and low formation damage rate.