Amaryllidaceae alkaloids have been isolated from the bulbs of Crinum ornatum and Crinum natans and studied by a combination of mass spectral techniques including EI, CI, FD and GLC/EI mass spectrometry. In addition to the abundant lycorine present in both species three new alkaloids have been obtained in crystalline form from C. ornatum and one new crystalline alkaloid from C. natans. Several other new alkaloids were also shown to be present by GLC/MS and FD/MS. Tentative structures are proposed for the new alkaloids from C. ornatum based on mass and NMR spectral evidence. Copyright © 1978 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim