New catalysts based on hydrotalcite-like precursors (Mg-Fe and Mg-Al-Fe) were synthesized. The structure of catalyst precursors was confirmed by XRD, FT-IR and TG. Appearance of separate brucite phase was observed for Mg-Fe precursors with excess of Mg, while for Mg-Al-Fe precursors, increase in Al content led to a formation of MgAl2(OH)(8) and mixed Al-Fe hydroxides apart from hydrotalcite phase. During calcination, the hydrotalcite like precursors spread their surface area and transform into mixed oxide. The mixed oxides were applied in ethylbenzene (EB) dehydrogenation with CO,. The activity losses with time-on-stream were completely restored by oxygen pulses.