Background: The quality of the dying experience among older adults should improve with a better understanding of the dying experience and its association with the place of death in Mainland China. Objective: This study investigated the relationship between the dying experience and place of death among older Chinese adults in the context of an urban-rural bifurcated system. Design: We used the end-of-life module data from the China Longitudinal Aging Social Survey conducted in 2014 and 2016 with an eligible sample of 352 decedents ages 60 and older. Facial expression and sadness at the end of life were indicators of the dying experience in the present study. We performed multiple regression models to examine the association between the place of death and dying experience after adjusting for an ecological array of factors at the individual, family, and community levels. Results: The urban-rural differences in the association between facial expression at death and place of death were identified (interaction term: β  = 0.16, p  = 0.004). Among the decedents with a rural residence status, dying in a hospital was associated with a more peaceful facial expression at death than dying at home (p  < 0.001). Among the decedents with an urban residence status, the place of death was not significantly related to the dying experience. Conclusion: Although home is perceived as a common place for death, the findings revealed that dying at home was less positive for rural older adults compared with dying in hospital. Bridging the gaps between urban and rural areas is necessary for the reform and construction of health care and long-term care systems in China.