In particle formation, the method can be just as important as the chemical reaction involved. A new method of synthesizing hydrotalcite-like layered double hydroxides (LDHs) of the type [Mg1-xAlx(OH)2]x+(CO32-)x/2·yH2O (x = 1.7−3.3) is reported. The key features of this method are a very rapid mixing and nucleation process in a colloid mill followed by a separate aging process. The properties of the resulting LDHs are compared with those of materials produced using the conventional coprecipitation process at constant pH. The compositions and structural parameters of the materials synthesized using the two routes are very similar, although the crystallinity is slightly higher for the LDHs produced using the new method. The thermal behavior of the materials synthesized using the two routes is also similar. The major advantage of the new method is that it affords smaller crystallites with a higher aspect ratio, having a very narrow distribution of crystallite size. In the conventional coprecipitation process at constant pH, the mixing process takes considerable time such that nuclei formed at the beginning of the process have a much longer time to undergo crystal growth than those formed at the end of the process. The consequence is that a wide dispersion of crystallite sizes is obtained. In the colloid mill process, however, the mixing and nucleation are complete in a very short time and are followed by a separate aging process. Furthermore, we suggest that the extreme forces to which the nucleation mixture is subjected in the colloid mill prevent aggregation of the nuclei and result in the nuclei having a uniform small size. When the resulting mixture is aged in a separate process, well-formed crystallites with a similarly narrow range of diameters result.