Nano-structured hydrotalcite-like compounds that contain nickel, cobalt and aluminum have been synthesized by conventional coprecipitation method without using any surfactants or templating agents. The structure and morphology of the coprecipitated nano hydrotalcites and its derived mixed oxides were characterized by powder X-ray diffraction (XRD), Fourier-transformed Infrared (FTIR) spectroscopy, field-emission scanning electron microscopy (FESEM), high resolution transmission electron microscopy (HRTEM), and nitrogen adsorption-desorption techniques. The results show that the synthesized materials exhibited micro-meso-pore networks. The cobalt-rich calcined hydrotalcites are generally amorphous, having a coral-like morphology whereas nickel-rich hydrotalcites show hexagonal plate-like morphology. The presence of nickel in mixed oxides catalyzed the reduction of Co-Al-O spinels. The Fast Fourier Transform (FFT) analysis of HRTEM revealed the inter planner distances of the crystal of hydrotalcite. © (2013) Trans Tech Publications, Switzerland.