In this article, the validity and accuracy of the CS-MT model introduced in article 1 for oil aggregates and in article 2 for nonionic surfactants is further evaluated by using it to model the micellization behavior of ionic and zwitterionic surfactants in aqueous solution. In the CS-MT model, two separate free-energy contributions to the hydrophobic driving force for micelle formation are computed using hydration data obtained from computer simulation: g(dehydr), the free-energy change associated with dehydration, and g(hydr), the change in the hydration free energy. To enable straightforward estimation of g(dehydr) and g(hydr) for ionic and zwitterionic surfactants, a number of simplifying approximations were made. Reasonable agreement between the CMCs predicted using the CS-MT model and the experimental CMCs was obtained for sodium dodecyl sulfate (SDS), dodecylphophocholine (DPC), cetyltrimethylammonium bromide (CTAB), two 3-hydroxy sulfonate surfactants (AOS-12 and AOS-16), and a homologous series of four DC(N)A bromide surfactants with a dimethylammonium head attached to a dodecyl alkyl tail and to an alkyl side chain of length C-N, having the chemical formula C12H25CNH2N+1N(CH3)(2)Br, with N = 1 (DC(1)AB), 2 (DC(2)AB), 4 (DC(4)AB), and 6 (DC(6)AB). For six of these nine surfactants, the CMCs predicted using the CS-MT model are closer to the experimental CMCs than the CMCs predicted using the traditional molecular-thermodynamic (MT) model. For DC(2)AB, DC(4)AB, and DC(6)AB, which are the most structurally complex of the ionic surfactants modeled, the CMCs predicted using the CS-MT model are in remarkably good agreement with the experimental CMCs, and the CMCs predicted using the traditional MT model are quite inaccurate. Our results suggest that the CS-MT model accurately quantifies the hydrophobic driving force for micelle formation for ionic and zwitterionic surfactants in aqueous solution. For complex ionic and zwitterionic surfactants where it is difficult to accurately quantify the hydrophobic driving force for micelle formation using the traditional MT modeling approach, the CS-MT model represents a very promising alternative.