Kafirin and zein could be used in making wheat-free leavened dough-based products if their functionality can be modified to more closely resemble gluten. Recently, stable viscoelastic masses were produced from isolated kafirin and total zein by dissolution of the prolamins in glacial acetic acid, followed by simple coacervation with rapid water addition. The methodology was, however, not compatible with food systems, as the final acid concentration was too high (33%). This work revealed that coacervation with reduction in the final acetic acid concentration down to 0.1% still enabled formation of kafirin and zein viscoelastic masses, with functionality retained on storage at 4 °C for an extended period; indicating an irreversible molecular change with dissolution in glacial acetic acid. Kafirin masses were much firmer than zein masses but both were softer than gluten. However, kafirin displayed a similarly elastic high component to gluten, whereas zein exhibited more viscous flow characteristics. This was probably due to the presence of more disulphide bonds in kafirin than zein. A model to explain this behaviour is proposed. Regarding the effect of prolamin concentration in glacial acetic acid, a minimum, between 5 and 10% was necessary for viscoelastic mass formation at low final acetic acid concentration (5%).