Seeds, of either commercial crucifer crops or some wild and weed relatives, were screened for intact glucosinolates using a previously developed ion-pair LC-MS method. This method, in contrast to GC-MS techniques, ensures the accurate measurement of all classes of glucosinolates. Many crucifer seeds contained very high concentrations of glucosinolates with low concentrations of additional pigments and secondary metabolites. The other common seed metabolites were cinnamoylcholine esters, for example, sinapine. Glucosinolates derived from homologues of l-methionine were characteristic of Brassica and related crucifer species. In addition, significant concentrations of 4-hydroxy-3-indolylmethylglucosinolate were found in the majority of Brassica species. Wild and weed species often had relatively simple glucosinolate profiles: either a single glucosinolate or a predominant glucosinolate together with trace amounts of others. Species identified with seed glucosinolate profiles suitable for purification included various Alyssum, Erysimum, and Iberis species for 3-methythiopropyl-glucosinolate and 3-methylsulfinylpropyl-glucosinolate and various Alyssum, Erysimum, and Lepidium species with very high concentrations of C4-C6 aliphatic glucosinolates. Seeds of Arabis, Barbarea, Lepidium, Moringa, and Sinapis species were good sources of aromatic glucosinolates, and Azima tetracantha was a good source for N-methoxy-3-indolylmethyl-glucosinolate. MS data are reported for all of the intact glucosinolates detected from the screening process.