The isolation and structure elucidation of the 17-membered macrocyclic spermine alkaloids (S)-verbasikrine (3), (S)-isoverbasikrine (6), (S)-verbamekrine (9), and (S)-isoverbamekrine (12) is presented. The syntheses of their racemates are described. The HPLC/APCI-MS analysis of the original total alkaloid extract of Verbascum pseudonobile is presented.