Abstract: Rehydration is shown to be straightforward for the reconstruction of polyoxometallate-pillared layered double hydroxides. Zn-Al hydrotalcite-like minerals were prepared with Zn/Al ratios of 1 to 5 by coprecipitation at pH 7. Good crystallinity was obtained for samples with Zn/Al ratios above 2. Thermal decomposition was achieved by calcining the samples at 300 to 900 °C. The calcined samples were exposed to decarbonated water, with or without hydrothermal treatment to evaluate reconstruction of the hydrotalcite-like minerals by rehydration. Restoration of the hydrotalcite-like structure was found to be independent of the Zn/Al ratios for samples calcined between 300 and 400 °C; however, a second phase, aluminum hydroxide or zinc oxide, was generally detected. A spinel phase, formed during the calcination of samples at temperatures above 600 °C, inhibited reconstruction of the hydrotalcite-like phase. The rehydrated hydrotalcite-like minerals had Zn/Al ratios close to 2, irrespective of the chemistry of the starting material.