Small unilamellar vesicles (∼100 nm in diameter) form spontaneously in aqueous mixtures of histidine and sodium dodecyl benzenesulfonate. By manipulating pH, a gradual transition from micelles to vesicles to bilayers to precipitate is observed. The self-assembly of vesicles occurs over a wide range of compositions when the solution pH is lower than 6.0, the pk a of the imidazole moiety on the histidine molecule. This phenomenon is likely the result of attractive interactions between the negatively charged benzenesulfonate headgroups and the positively charged imidazole group in the amino acid. Similar results are obtained when imidazole salt itself is used.