The free-floating bike-sharing system (FFBS) is an innovative public bicycle service, which is widely popular throughout China. In comparison to traditional station-based system, FFBS allows cyclists to park the bicycles in any non-motorized parking area so that the convenience can be improved greatly. Moreover, smart devices inside the free-floating bicycle can provide real-time tracking information which offers convenience for intelligent management. This study adopts the structural equation model to measure what factors influence people’s willingness to use the system and how the indicators inside the system interact with each other. Unlike the long-standing use of maximum likelihood estimation method, an approach of partial least squares estimation is used in this paper to remove the restriction of multivariate normal distribution. Based on the questionnaire carried out in 32 locations in Shanghai, a conceptual framework cyclist satisfaction index model is established, which includes three levels with 50 indicators. Then, to analyze the different perception among different kinds of cyclists, the study divides them into two groups: commuters and non-commuters. The parameter calibration for commuters and non-commuters are calculated separately. Finally, by virtue of importance-performance analysis (IPA) matrices, the problems in the existing service system are identified. The results demonstrate five aspects including riding environment, riding safety, government intervention, laws and staff service need urgent improvement. According to these findings, innovative countermeasures such as monitoring platform and electronic fences are under construction to prompt the use of FFBS.