It is shown that the addition of sodium dodecyl sulfonate (SDS) greatly enhances the dewatering performance at high temperatures of alumina model mineral suspensions to which poly(N-isopropylacrylamide) (PNIPAM) has been added as a temperature responsive flocculant. Batch settling tests have been conducted showing the enhancement of settling rates and supernatant clarity with the binary surfactant system. Micropolarity and flotation tests were undertaken to demonstrate the increased relative micro- and macro-phase hydrophobicity of the PNIPAM/SDS/Alumina systems. Electroacoustic studies were used to show that the decrease in zeta-potential in the PNIPAM/SDS/Alumina system is predominantly a function of SDS concentration rather than the presence of PNIPAM above its phase transition temperature. Adsorption studies illustrated not only that the adsorption of PNIPAM onto the alumina increases with SDS concentration for all temperature treatments but that a corresponding reduction in the desorption of PNIPAM after lowering the equilibration temperature is observed. From these investigations a mechanism of mineral oxide suspension separations with a binary surfactant system is proposed. An understanding of the means and mechanisms through which co-surfactants can be used to aid settling of PNIPAM-derivative flocculated mineral systems is important for the targeted development and application of intelligent polymers to solid-liquid separations.