In order to research the high-concentration CO2 effects on ignition delay time (IDT) of diesel surrogate fuel (70% n-heptane/30% toluene), a carbon dioxide effect (CDE) model is established, which considers fuel and ambient gas concentration, density, and temperature influence on autoignition under CO2/O2 atmosphere. Firstly, a chemical model of n-heptane/toluene is established, and the coupling, reduction, and simulation processes are carried out in chemical kinetic software with the IDT as the target parameter. Secondly, a constant volume combustion chamber (CVCC) visualization platform is built by incorporating a high-speed camera system and different working conditions are set in the CO2 volume fraction range (40%-70%) at 3.0 MPa and 850 K for an autoignition experiment. Thirdly, experiment and simulation results are discussed in air, 60% CO2/40% O2, 50% CO2/50% O2, and 40% CO2/60% O2 atmospheres, including the IDT, CO2 effects, temperature sensitivity, and OH radical rate of production (ROP). The results show that the CDE model well predicts the 70% n-heptane/30% toluene IDT under the CO2/O2 atmosphere and the average error in 60% CO2/40% O2 atmosphere is 5.29%. Besides, when the CO2 volume fraction increases from 40% to 60%, the CO2 thermal effect plays a leading role in the IDT prolongation and the OH radical ROP peak of R4 (O+H2O⟶2OH) decreases by 180%.