This study investigated dye-surfactant interactions between a series of modified Gemini surfactants and commercial direct dyes in aqueous solution and their corresponding effects on cotton fabric dyeing. A surface tension meter was also used to measure surface activities of compounds containing electrolyte under conditions similar to those in dyeing processes. The surface tension measurements showed lower than normal surface tension in surfactant solutions containing electrolyte. From the UV-Vis spectra, the isosbestic point indicated that dye-surfactant complexes had formed and existed as hydrophilic interaction between direct dyes and modified Gemini surfactants. When dyeing cotton fabric with red dye and orange dye, the presence of these surfactants decreased dye uptake rate but increased for blue dye because the dye-surfactant interaction had formed a hydrophilic complex.