The effects of various parameters of synthesis on the structure formation of layered double hydroxides (LDH) of the general formula M3Al(OH)8[(CO3)1/2 · mH2O], where M = Zn2+, Mg2+, or Cu2+, were studied. The possibility of modifying LDH in order to expand the interlayer spacing was demonstrated. The behavior of the obtained samples on heating was studied by thermal analysis. The qualitative composition was confirmed by X-ray powder diffraction (XRD). The structure was studied by scanning electron microscopy (SEM).