Functional photoluminescent materials are emerging as a fascinating subject with versatile applicability. In this work, luminescent organic-inorganic hybrid hydrogels are facilely designed through supramolecular self-assembly of sodium cholate, and lanthanide ions such as Eu(3+), Tb(3+), and Eu(3+)/Tb(3+). Fluorescence microscopy and TEM visualization demonstrates the existence of spontaneously self-assembled nanofibers and 3D networks in hybrid hydrogel. Photoluminescence enhancement of lanthanide ions is realized through coordination with cholate and co-assembly into 1D nanofibers, which can successfully shield the Eu(3+) from being quenched by water. The photoluminescence emission intensity of a hybrid hydrogel exhibits strong dependence on europium/cholate molar ratio, with maximum emission appearing at a stoichiometry of 1:3. Furthermore, the emission color of a lanthanide-cholate hydrogel can be tuned by utilizing different lanthanide ions or co-doping ions. Moreover, photoluminescent lanthanide oxysulfide inorganic nanotubes are synthesized by means of a self-templating approach based on lanthanide-cholate supramolecular hydrogels. To the best of our knowledge, this is the first time that the lanthanide oxysulfide inorganic nanotubes are prepared in solution under mild conditions.