Along with reducing traffic congestion, electric car-sharing (ECS) can also solve travel demand, utilize idle resources, and enhance forms of transportation. Accordingly, university students are identified in Guangzhou, China as a promising customer group for ECS companies. Although university students in Guangzhou, China are unique in the context of ECS, few researchers have studied the factors that influence their willingness to use such services. Hence, this paper investigates the key determinants that affect university students’ behavioral intention (BI) to use ECS in Guangzhou, China. Based on an extension of the unified theory of acceptance and use of technology (UTAUT), this paper examines the effects of the constructs on BI to use ECS and the moderating role of trust in ECS. Based on results from a questionnaire of 486 university students in Guangzhou, China, conditional value (CV) was the most critical driver of BI, followed by personal attitude (PA) and sustainability (SUST). The moderating analysis showed that taking gender, education, and driving experience of university students as control variables, trust was found to have a significant positive moderating impact on the relationship between PA and BI to use ECS, and a significant negative moderating effect of trust on the relationship between CV and BI to use ECS. The implications of these findings are discussed.