The influence of ionic and nonionic surfactants on the solubility, nucleation, and growth habit of γ-aminobutyric acid (GABA) in water has been studied. Between 25° and 55 °C, no effect of the surface-active agents on GABA solubility was detected. On the other hand, it has been found by two experimental techniques (laboratory-scale batch crystallization and DSC), that these additives tend to delay homogeneous nucleation. Attachment energies of the main crystallographic faces of GABA (F faces in the PBC theory) were calculated via molecular/crystal modeling by means of the GenMol software, in order to rpedict the theoretical habit of GABA crystal in vacuo. Predictions on habit modification are found in good agreement with the shape of crystals grown from aqueous solution with or without additive.