Bike-share systems are proliferating across the US and could expand opportunities for those most underserved by the transportation system. A deeper understanding of current bike-share users could enable the expansion of these services and their benefits to a larger population. With the aim of deepening this understanding, this study uses data from household and bike-share user surveys in the Sacramento region to perform behavioral modeling and market segmentation. The results show that although individuals with low incomes and students are less likely than other demographic groups to use bike-share, they use it more frequently if they do use it. Individuals who regularly use multiple modes of travel also use the service frequently. The initial adoption of the service by transport-disadvantaged groups can play a vital role in the continued and frequent use of the service. The market segmentation analysis shows that low-income individuals, students, and zero-car individuals use the service frequently for commuting and a variety of non-commuting purposes. The occasional users of the bike-share service are mainly those with higher incomes and individuals who have access to a personal car. Another market segment consists of non- and infrequent-personal bike users; however, that segment is using the bike-share service at a greater rate for different purposes compared to regular bicyclists. This suggests that bike-share may fill an important travel gap and act as a lever for increasing bike travel for some users. Overall, the results provide detailed bike-share market information that can be used to tailor urban transport policies. The results also suggest that if the user base for bike-share programs were expanded to reach even more low-income individuals, students, and multi-modal travelers, greater environmental sustainability benefits would be achieved.