Organic-inorganic layered double hydroxides (LDHs) were obtained by using a microwave-assisted method to intercalate cholate or deoxycholate ion into an Mg, Al mixed LDH. Based on the X-ray diffraction and Raman spectra for the resulting LDHs, a treatment time of only 1 h sufficed to ensure complete intercalation of the organic anions. This makes the proposed synthetic method more expeditious than existing alternatives for the same purpose. Based on the baseline spacing for the organo-LDHs, the organic anions were intercalated with no cross-over between their molecular chains. The interlayer distance of the solids was confirmed by high-resolution transmission electron micrographs (HR-TEM). As revealed by thermogravimetric monitoring measurements, and confirmed by Raman spectra, the decomposition temperature for the LDHs increased considerably upon intercalation of the organic anion.