Solutions of sodium dodecyl benzene sulfonate (SDBS) and N,N-dimethyldodecan-1-amine oxide (DDAO) with mole fractions of 0.00, 0.25, 0.50, 0.75 and 1.00 were prepared and their surface tension was measured as a function of total surfactant concentration. The critical micelle concentration (CMC) values of these mixed solutions were also determined. The minimum area occupied by a surfactant molecule at air/water interface was calculated for single and binary surfactant mixtures. A pronounced synergistic interaction between SDBS and DDAO was detected. The surface tension and CMC-values of SDBS/DDAO mixtures are significantly lower than those of the single surfactant. The mixed system of SDBS/DDAO exhibits a highly negative interaction parameter (β = −10.6) according to regular solution model, and is found to fulfill the condition of Hua and Rosen, indicting a strong synergistic interaction between the two surfactants. The contact angle measurements show the wettability of the surfactant mixture onto polyethylene substrate is higher than of the respective single surfactant. In addition, the adsorption of SDBS and DDAO or their mixtures on 1.0% activated carbon and 5.0% Jordanian natural clay (JNC), respectively, was investigated using the depletion method. The individual surfactants were found to adsorb to a considerable extent on activated carbon, and a slightly higher adsorption tendency was even measured for mixed SDBS/DDAO surfactant systems. Although no SDBS molecules adsorbed on JNC, adsorption was observed for solutions containing DDAO and SDBS/DDAO surfactants. The improvement in wettability and adsorption of SDBS/DDAO surfactants at the air/water and solid/water interfaces is directly related to the synergistic interaction between the two surfactants.