Three new dimeric cholesterol-based compounds of A(LS)(2) type, where A stands for aromatic component, S steroid moiety, and La linker connecting the two units, have been designed and prepared. Gelation test in 30 solvents demonstrated that the compounds can gel some of the solvents and form 37 gels, of which 16 form spontaneously at room temperature (similar to 25 degrees C). These gels possess smart thixotropic properties as revealed by rheological studies. FTIR and H-1 NMR measurements revealed that hydrogen bonding is an important driving force for the formation of the gel networks. XRD analysis demonstrated that unlike commonly found layered structures adopted by dimeric cholesterol-based low-molecular mass gelators (LMMGs), one of the gelators created in this study adopts a hexagonal packing structure in its benzene gel. (C) 2011 Elsevier Inc. All rights reserved.