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