Drug-loading mesoporous silica nanoparticles that serve as a nanoreservoir-type drug-delivery system are successfully attached to titanium substrates via the layer-by-layer assembly technique (see scheme). The obtained structure demonstrates great potential for regulating the biological behaviors of osteoblasts/steoclasts in order to maintain bone homeostasis. The approach we present here may have wide applications in implant technology, tissue engineering, and regenerative medicine.