The Australian family Gyrostemonaceae, comprising 17 species in 5 genera, has lately attracted much taxonomic interest [1]. In 1950, (+)-2-butyl isothiocyanate (2) was identified as a volatile constituent of fresh leaves of Codonocarpus cotinifolius (Desk) F. Muell. [2], a finding to which systematic significance has been attributed in a recent discussion [1]. We report the occurrence of 2-propyl- (4), 2-butyl- (5) and 2-methylpropyl-glucosinolate (6) in seeds and leaves of Tersonia breuipes Moq., another member of Gyrostemonaceae, collected in the wild in West Australia. On myrosinasecatalysed hydrolysis, 2-propyl (1), 2-butyl (2) and 2 methylpropyl isothiocyanate (3), were produced from the glucosinolate mixture in seeds as well as dried leaves, with (1), in both cases, accounting for about 90 % of the isothiocyanate fraction. The enantiomeric composition of the chiral isothiocyanate (2) has not been established. The finding of glucosinolates in a second member of the Gyrostemonaceae lends support to the suggested affinity of the family to those enclosed in the order Capparales [1]. It is notable that the glucosinolates encountered so far are biogenetically derived from protein amino acids, viz. valine, isoleucine and leucine, and not from their homologized counterparts (cf. ref. [5]). On this count, Gyrostemonaceae may be assigned primitive ordinal rank.