Mg-Zn-Ca bulk metallic glass (BMG) is a promising orthopedic fixation implant because of its biodegradable and biocompatible properties. In recent years, the structural supporting bone implants with osteo-induction property for effective bone regeneration are highly desired. Osteogenic growth peptide (OGP) can not only increase the proliferation as well as differentiation in mesenchymal stem cells, but enhance the mineralization in osteoblast cells. However, the short half-life and non-specificity to the target area limit the application of OGP. Mesoporous silica nanoparticles (MSN) as nanocarriers possess excellent properties such as easy surface modification, superior targeting efficiency, and high loading capacity of drugs or protein. Accordingly, we propose a system of combining the OGPcontained MSN with Mg-Zn-Ca BMG materials to promote bone regeneration. In this work, we conjugated cysteine-containing OGP (cgOGP, 16 a.a.) to the interior walls of the channels in MSNs and maintained the MSNs’ dispersity via pegylation. In vitro study showed that the released metal ions from the degradation of Mg-Zn-Ca BMG could promote cell proliferation and migration as well as elevate the ALP activity and mineralization. Despite the planned MSN (without OGP) showed little inhibition in cell migration and mineralization, superior results were obtained while treating cells simultaneously with the BMG ion-contained MEM and OGP-conjugated MSN. This result was contributed by the controlled released of OGP via enhancing the focal adhesion turnover and promoting the differentiation. Hematological analysis also confirmed the biocompatibility of this BMG/nanocomposite system. In addition, in vivo micro-CT and histological observation revealed that our system stimulated the osteogenesis and new bone formation around the implant site.