This chapter describes a mixed-method, multiple case study that examined ways in which synchronous educational Twitter chats were used, first, to enhance graduate and undergraduate university student learning, second, to build professional networks, and third, to provide a loosely regulated means to achieving self-determined professional development goals. Findings suggest that while difficult at the onset, participation in Twitter educational chats was an enhancement to students’ overall course learning experience. Specifically, university students’ use of chats for educators helped them achieve social presence in this virtual environment, as well as to better understand the connections between positive student-teacher relationships and K12 student learning. Included are recommendations for use of Twitter synchronous educational chats in the college classroom as well as future directions in research.