With the emphasis on sustainability in transportation, bike-sharing systems are gaining popularity. This paper investigates the attitudes of users of a bike-sharing system with the aim of identifying their priorities, thus allowing local governments to focus their efforts most effectively on enhancing users’ intentions to use such systems. The relationships among green perceived usefulness (the extent to which individuals believe that a bike-sharing system will improve the environmental performance of some part of their life within a specific context), user attitude and perceived ease of use with green intentions, and the mediation effect of user attitude towards bike-sharing are explored. The focus of the study is on how to enhance green intentions via perceived usefulness, perceived ease of use and user attitude of the green technology acceptance model (green TAM) (Davis 1989). The two-step approach of structural equation modeling was applied to analyze the empirical results, which indicated that green perceived usefulness and user attitude have positive influences on the green intentions of 262 users and 262 non-users from ten sampled bike-sharing sites around the central administrative districts of Taipei. However, user attitude has the highest mediation effect on green intentions, and perceived ease of use does not have a significant effect on intentions for either users or non-users. Therefore, governmental institutions can strive to improve the attitudes of bike-sharing users and non-users, their green perceived usefulness, and perceived ease of use to strengthen their intentions to use this mode of sustainable transportation.