Two new pyrrolizidine alkaloids, namely, neocroalbidine and neocroalbidinone, were isolated from the herbs of Crotalaria albida. Their structures were established using a combination of NMR spectroscopy and mass spectrometry techniques. The absolute stereochemistry of the two alkaloids presented herein was determined by single-crystal X-ray diffraction analysis. Crown Copyright (C) 2013 Phytochemical Society of Europe. Published by Elsevier B.V. All rights reserved.