As important unit for regional health planning, urbanized counties are facing challenges because of internal migrants and aging. This study took urbanized counties in China as cases and two key populations as objects to understand different populations’ intentions of choosing corresponding health service resources and to provide support for resource allocation. A cross-sectional study was conducted in Kunshan, a highly urbanized county in China, in 2016, among older adults aged 60 or over and children aged 0–6. Multinomial logistics models were used to identify the factors associated with healthcare choices. In this study, we found that income, distance of the tertiary provider, and migrant status were not associated with choices of tertiary healthcare outside county for children, while parents’ education level was. The responsiveness of the tertiary provider inside the county was lower than primary and secondary providers inside the county, while respondents were dissatisfied with the medical technology and medical facility for the tertiary inside the county compared to those of the tertiary provider outside the county. Significant differences existed in terms of the perception of different categories of institutions. To conclude, local governments should particularly seek to strengthen pediatric primary health services and improve the responsiveness of healthcare facilities to treat geriatric and pediatric diseases, which also bring significance to the developing countries in the process of urbanization.