Here, we present experimental surface-tension isotherms of mixed solutions of two surfactants, sodium dodecyl sulfate (SDS) and cocoamidopropyl betaine (Betaine), measured by means of the Wilhelmy plate method. The kinetics of surface-tension relaxation exhibits two characteristic time scales, which have been distinguished to determine correctly the equilibrium surface tension. The transition from the zwitterionic to the cationic form of Betaine is detected by surface-tension measurements. Synergistic dependence of the critical micellization concentration on the composition of the surfactant blend is established. The experimental surface-tension isotherms are fitted by means of the two-component van der Waals model, and an excellent agreement between theory and experiment was achieved. Having determined the parameters of the model, we calculated different properties of the mixed surfactant adsorption layer at various concentrations ofSDS, Betaine, and salt. Such properties are the adsorptions ofthe two surfactants, the surface dilatational elasticity, the occupancy of the Stern layer by bound counterions, the surface electric potential, and so forth. In particular, the addition of a small amount of Betaine to SDS significantly increases the surface elasticity. The results could be further applied to predict the thickness and stability of foam films or the size of the rodlike micelles in the mixed solutions of SDS and Betaine.