The traditional method of designing freeway geometric characteristics may not well consider traffic safety and evaluation problems associated with vehicle, driver, road, and environmental features. This paper looks into accident-prone compound curves and puts forward a traffic safety evaluation method that can comprehensively assess various influencing factors. This method integrates driving simulation and Virtual Reality (VR) technology. Methodically, this paper first used three-dimensional (3D) design software to build the digital model and spatial scene model of the compound curves from the aspects of geometric structure, spatial characteristics, terrain information, and so on. Next, drivers were invited to conduct a series of driving simulation experiments upon the human–computer interaction safety experience platform, and driver physiological data and vehicle driving information collected. Last but not least, the mean values of heart rate changes, steering wheel angle changes, and driving trajectory changes were derived to synthesise the comprehensive traffic safety evaluation framework. Based on the analysis of the results of the orthogonal test, select the road plane design indicators that have a significant impact on the traffic safety evaluation, and carry out regression analysis. The research shows that the novel traffic safety evaluation method integrating with VR technology can comprehensively consider various influencing factors, and designers can dynamically adjust the design metrics according to the traffic safety level.