Glioblastoma is one of the most lethal cancers with few available therapeutic options. Herein, we report a in situ self-assembled nanoplatform formed by RGD peptide-modified Bisulfite-ZincII-Dipicolylamine-Arg-Gly-Asp (Bis(DPA-Zn)-RGD) and ultrasmall Au-ICG nanoparticles. Taking advantage of RGD-mediated neovascular targeting, the Bis(DPA-Zn)-RGD selectively navigates to the tumor site, and then assembles into large nanoclusters with subsequently administered Au-ICG nanoclusters which can successfully cross the BBB due to ultrasmall particle size (~7 nm). This study demonstrates that such in situ self-assembly metal–organic nanosystems are ideal to overcome the BBB and BBTB, which promise a new way for orthotopic brain tumors imaging and therapy.
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