The surface properties of some families of cationic two-headed surfactants based on a pentaerythritol backbone are described. The compounds have the following general structure (1), where R' are head groups and R are linear alkyl groups ranging from octyl to tetradecyl. The syntheses of these compounds has been published in detail previously. Critical micelle concentrations (cmc values) of these two-headed surfactants have been determined and compared to conventional ionic surfactants and gemini surfactants of similar structure. In addition, the surface activity of these two-headed surfactants, expressed as the C-20 value and the surface tension at the cmc, have been determined. Transmission electron microscopy has been used to examine the morphology of the aggregates formed by these amphiphiles. In general, when compared to conventional ionic and two-headed surfactants, these new two-headed surfactants exhibit a remarkable efficiency in the tendency to self-assemble and are significantly more surface active than their conventional counterparts. [GRAPHICS] (C) 2014 Elsevier Inc. All rights reserved.