A phytochemical study on Borreria verticillata has led to the isolation of two novel simple indole alkaloids, 6-methoxy-4-(3-methylbut-2-en-1-yl)-1H- indole, named verticillatine A (1), and 1-(1H-indol-6-yl)-3-methylbutan-1-one, named verticillatine B (2), one new iridoid, 6′-O-(2-glyceryl)scandoside methyl ester (3), with the glycerol unit linked to a glucose unit, and two known ones, asperuloside (4) and scandoside methyl ester (5). The structures of these compounds were elucidated on the basis of spectroscopic-data analyses, mainly 1H- and 13C-NMR, including 2D experiments ( 1H,1H-COSY, NOESY, HMBC, and HMQC), and HR-ESI-MS. © 2010 Verlag Helvetica Chimica Acta AG.