Mg-Al, Zn-Al, and Mg-Fe layered double hydroxides (LDHs) have been synthesized through a stepwise control route. In the stepwise control route, we controlled the state of Al or Fe composition as Al or Fe hydroxyl aqueous complexes in aqueous solution first, then dropwise Mg2+ or Zn2+ and OH - and keep procedure at constant pH value simultaneously at room temperature. The textural and structure properties of the resulting samples were characterized by XRD and TG-DTG. The results showed that products obtained by the stepwise control route were pure and highly crystalline LDHs. The particle size and size distribution was measured by DLLS.