A method of making silica-layered double hydroxide microspheres having the formula I: (i) wherein, Mz+ and M′y+ are two different charged metal cations; z=1 or 2; y=3 or 4; 0 0, q>0, Xn− is an anion; with n>0 a=z(1−x)+xy−2; and the AMO-solvent is an 100% aqueous miscible organic solvent; comprises the steps: (a) contacting silica microspheres and a metal ion containing solution containing metal ions Mz+ and M′y+ in the presence of a base and an anion solution; (b) collecting the product; and (c) optionally treating the product with AMO-solvent and recovering the solvent treated material to obtain the silica-layered double hydroxide microspheres. Preferably, M in the formula I is Li, Mg, Ni or Ca. Preferably, M′ in formula I is Al. The invention further provides silica-layered double hydroxide microspheres having the formula I. The silica-layered double hydroxide microspheres may be used as catalysts and/or catalyst supports. (SiO2)p@{[Mz+(1-x)M′y+x(OH)2]a+(Xn−)a/n.bH2O.c(AMO-solvent)}q  (I)