Gelation behavior of lithocholate (LC(-)) mixed with different monovalent cations in water was detected. The hydrogels consisting of tubular networks were formed by introducing alkali metal ions and NH4(+) to lithocholate aqueous solutions at room temperature. The formation of tubular structures was considered to be mainly driven by the electrostatic interaction with the assistance of a delicate balance of multiple noncovalent interactions. It is interesting that the increase in temperature can induce a significant enhancement in strength of the hydrogels, accompanied by the formation of bundles of tubules and larger size aggregates. The mechanism of the temperature-induced transition can be explained by the "salting-out" effect and the electric double layer model. The hydrogels showed very high adsorption efficiency and adsorption capability for the cationic dyes and were promising to act as toxic substance adsorbents.