A novel cancer-cells-triggered controlled-release gadolinium-doped luminescent and mesoporous strontium hydroxyapatite nanorods (designated as Gd:SrHap nanorods) system using cell-type-specific aptamers as caps has been constructed. Aptamers behave as a dual-functional molecule that acts as not only a lid but also a targeted molecular that can be used in an effective way for therapeutically special cancer cells. After incubated with cancer cells, for example, MCF-7 cells, the doxorubicin-loaded and aptamer-capped Gd:SrHap nanorods (designated as Gd:SrHap-Dox-aptamer) can be internalized into MCF-7 cells, resulting in the pore opening and drug releasing. Furthermore, the high biocompatibility and biodegradability Gd:SrHap nanorods with blue autofluorescence and paramagnetism could serve as a good contrast agent of targeting fluorescence and magnetic resonance imaging. We envision that this Gd:SrHap system could play a significant role in developing new generations of site-selective, controlled-release delivery and interactive sensory nanodevices.