The use of urea as a precipitating agent in the synthesis of Ni-Al and Zn-Al layered double hydroxides having a hydrotalcite-like structure via a microwave-hydrothermal method is reported. For comparison purposes, the samples were also prepared by a conventional hydrothermal method. Ni-Al compounds with the hydrotalcite-like structure were obtained in shorter periods of time by the microwave method than by the conventional method, whereas when zinc cations were involved, no successful synthesis was achieved regardless of the method used. In order to find the best synthesis conditions for the Ni-Al solids, samples were submitted to microwave-hydrothermal treatment at different temperatures for increasing periods of time, and the structural, thermal, and textural properties of the synthesized materials were evaluated. All of the solids were fully characterized by chemical elemental analysis, powder X-ray diffraction (PXRD), FT-IR spectroscopy, and transmission and scanning electron microscopy as well as by N-2 adsorption/desorption at -196 degrees C for assessment of specific surface area and porosity. The PXRD patterns showed that the layered structure appeared after merely 10 min when the synthesis was carried out at 125 degrees C; however, the FT-IR spectra showed the presence of some cyanate groups that were formed during urea hydrolysis and were quite difficult to remove completely. When the conventional hydrothermal treatment was used, longer periods of time were required in order to develop the hydrotalcite-like structure, but increasing the aging time improved the crystallinity of the compounds and yielded large particles.