To explore the phytochemistry of the African ethnomedicinal plant Cryptolepis sanguinolenta (Lindl.) Schltr. (Apocynaceae) for rare indoloquinoline alkaloids, two novel indoloquinoline alkaloid glycosides, namely Cryptospirosanguine A (1) and B (2), were isolated from an ethanolic extract of the root. Their structures were elucidated based on spectral evidence. Furthermore, two known terpenoids were isolated from this plant for the first time.