Supramolecular hydrogels were prepared in the mixtures of a chiral amphiphilic lithocholic acid (LCA) and a nonionic surfactant, dodecyldimethylamine oxide (C(12)DMAO), in water. With the addition of LCA to C(12)DMAO micellar solutions, a transition from micelles to gels occurs at room temperature. Hydrogels can form at very low concentrations (below 0.1 wt %), exhibiting a super gelation capability. The rheological measurements show a strong mechanical strength with an elastic modulus exceeding 5000 Pa and a yield stress exceeding 100 Pa. Microstructures determined by TEM, SEM, and AFM observations demonstrate that the gels are formed by intertwined helical fibrils. The formation of fibrils is induced by enormous cycles of units composed of two LCA molecules and four C(12)DMAO molecules driven by comprehensive noncovalent interaction, especially the hydrogen bonds produced in two reversed LCA molecules and the C(12)DMAOH(+)-C(12)DMAO pairs. The xerogels show excellent adsorption capability of the toxic dye with a maximum adsorption value of 202 mg.g(-1).