While great progress in the development of a methodological approach to measure the accessibility of healthcare services has been made, the exclusion of the complex multi-mode travel behavior of urban residents and a rough calculation of travel costs from the origin to the destination limit its potential for making a detailed assessment, especially in urban areas. In this paper, we aim to describe and implement an enhanced method that enables the integration of multiple transportation modes into a two-step floating catchment area (2SFCA) method to estimate accessibility. We used a travel-mode choice survey, based on distance sections, to determine the complex multi-mode travel behavior of urban residents. Taking Nanjing as a study area, we proposed complete door-to-door approaches to determine every aspect of basic transportation modes. Additionally, we processed open data to implement an accurate computing of the origin-destination (OD) time cost. We applied the enhanced method to estimate the accessibility of residents to hospitals and compared it with three single-mode 2SFCA methods. The results showed that the proposed method effectively identified more accessibility details and provided more realistic accessibility values.