Underground spaces hold significant potential for enhancing urban resilience against disasters, a key dimension of sustainable urban development. However, due to persistent associations of underground environments with negative psychological perceptions, these spaces—despite their superior protective advantages—are often overlooked as viable refuge options during emergencies. Guided by the theoretical framework of environmental psychology, this research focuses on underground parking garages in Hangzhou, China as its primary research object. The target participants are residents of Hangzhou aged 18–58 years (encompassing diverse occupations such as students, office workers, and service industry employees), who represent potential users of such spaces as refuges. To explore human behavioral patterns, psychological responses, and needs related to underground refuge spaces, we employed a two-phase methodology: first, a questionnaire survey to capture broader behavioral tendencies and subjective perceptions; complementing this, Virtual Reality (VR) experiments—a more immersive method—utilizing semantic analysis and the Likert scale to assess psychological indicators influenced by underground environments. The experimental data were analyzed via mean analysis, correlation analysis, and multiple linear regression analysis to identify the key environmental factors that influence psychological responses, as well as their optimal design parameters. These analyses reveal significant correlations between various environmental factors and psychological indicators. This research synthesizes individuals’ psychological tendencies in underground environments and proposes quantitative physical design guidelines to meet fundamental psychological needs. The findings provide theoretical and practical support for the design of underground space for refuge and the development of sustainable urban emergency shelter systems, thereby contributing to resilient and sustainable urban development.