We demonstrate an efficient synthesis of novel layered double hydroxide mesoporous silica core-shell nanostructures (LDH@mSiO(2)) that have a hexagonal MgAl-LDH nanoplate core and an ordered mesoporous silica shell with perpendicularly oriented channels via a surfactant-templating method. Transmission electron microscopy, X-ray diffraction and N(2) sorption analyses confirmed that the obtained nanostructures have uniform accessible mesopores (∼2.2 nm), high surface area (∼430 m(2) g(-1)), and large pore volume (∼0.22 cm(3) g(-1)). Investigations of drug release and bio-imaging showed that this material has a slow release effect of ibuprofen and good biocompatibility. This work provides an economical approach to fabricate LDH@mSiO(2) core-shell nanostructures, which may have great potential in broad drug delivery and hyperthermia therapy applications.