Layered double hydroxides(LDHs) with hydrotalcite-type structure containing Fe3+, Al3+ and Mg2+ were prepared by means of a coprecipitation method. The products were characterized by element analysis, X-ray powder diffraction and transmission electron microscopy. It was found that even if the molar ratio of n(Fe+Al)/n(Fe+Al+Mg)>0.33, yet a pure hydrotalcite-like compound(HTlc) phase was gained when n(Fe)/n(Al+Mg+Fe)≤0.30 and n(Al)/n(Al+Mg+Fe)≤0.30; the Al(OH)3 phase appeared in the products when n(Al)/n(Al+Mg+Fe)>0.30; and an amorphous phase emerged when n(Fe)/n(Al+Mg+Fe)>0.33. These results show that there is no concentration superposition effect between Fe3+ and Al3+ on the crystalline state of the produced samples. In our previous work, the concentration superposition effect between Zn2+ and Mg2+ in the synthesis of Zn-Mg-Al-LDHs was found. For the prepared Fe-Al-Mg-LDHs samples, the value of lattice parameter a is between 0.30-0.32 nm; and the value of lattice parameter c is between 2.30-2.47 nm, the basal spacing is in the range of 0.76-0.83 nm. When the ratio of n(Fe)/n(Al) is a constant, the values of a and c increase with the increase of the Mg2+ content of the produced samples. The mean particle size and the mean crystal grain were determined by virtue of a particle-size instrument, XRD-Scherrer formula and TEM method, respectively.