A multi-nanoparticle-embedded amorphous aluminum/magnesium oxides (AAMO) core/mesoporous silica (mSiO(2)) shell structure has been successfully synthesized by calcining the presynthesized catalyst precursor-containing layered double hydroxide (LDH) core/mesoporous silica shell composite. The well-dispersed catalytic nanoparticles were fixed at the interface between AAMO core and mesoporous SiO2 shell, i.e., at the inner pore mouths of the mesoporous SiO2 shell, which could effectively prevent nanoparticles from growth and/or aggregation with each other and in the meantime allow efficient access of reactants to the catalytic NPs. The final core/shell composite was found to be an efficient and highly recyclable heterogeneous catalyst.