The pyrroloindoline alkaloids are a structurally diverse family of biologically active natural products, which include compounds such as hodgkinsine (1), naseseazine A (2), and gliocladine C (3) 3 (Fig. 1). As a result of their compelling bioactivities and fascinating structures, this family of alkaloids has been the subject of intense research and has inspired the development of a variety of n...