Recruiting endogenous stem cells and achieving controlled drug release are crucial for in situ bone regeneration. However, it remains challenging to design functional platforms that can effectively recruit stem cells and deliver drugs at an appropriate dose and a time-dependent manner under specific stimulus conditions. Herein, mesoporous bioactive glass (MBG), nanoreservoirs of the simvastatin (Sim), was end-capped with E7 peptide-modified gold nanoparticles (Au-NPs). This unique design allowed for effective recruitment of endogenous stem cells and enabled the sustained release of simvastatin. The released simvastatin facilitated the osteogenic differentiation of stem cells, supporting bone-like tissue reconstruction. Meanwhile, under near-infrared light irradiation, MBG@Sim-Au-E7 exhibited adaptive degradation and sustained release of simvastatin and active ions. This capability regulated the osteogenic microenvironment, further facilitating bone regeneration. In addition, the results of in vivo experiments showed that the healing of skull defect was significantly improved by MBG@Sim-Au-E7 after NIR irradiation. These findings highlight the potential of MBG@Sim-Au-E7 as a promising approach for preparing functional bone healing materials.