Plants of the Aconitum, Delphinium, and Consolida genera are recognized as rich sources of biologically active and structurally complex diterpenoid alkaloids. In this paper we report on the structure of cardionine (1) and 11-acetylcardionine (2), new C20-diterpenoid alkaloids isolated from Delphinium cardiopetalum DC and D. gracile DC, respectively, using the Selective INAPT NMR Technique. 11-Acetylcardionine (2) had a molecular formula C25H35NOS determined by HREIMS. Its 1H and 13C NMR spectra, among other characteristic features of a C20-diterpenoid alkaloid with a hetisine-type skeleton.