Integration of clinical imaging and collaborative multimodal therapies into a single nanomaterial for multipurpose diagnosis and treatment is of great interest to theranostic nanomedicine. Here we report rational design of a discrete Os-based metal-organic nanocage Pd6(OsL3)828+ (MOC-43, L = (2-(pyridin-3-yl)-1H-imidazo[4,5-f][1,10]-phenanthroline ligand) which can act as a versatile theranostic nanoplatform to meet the following demands simultaneously: 1) synergistic treatments of radio-, chemo- and X-ray induced photodynamic therapies (X-PDT) for breast cancer, 2) NIR orthotopic imaging for cancer cell tracking and tumor-targeting, and 3) anticancer drug transport through a host–guest strategy. The nanoscale MOC-43 incorporates eight high-Z Os-elements to interact with X-ray irradiation for dual radiosensitization and photosensitization, showing efficient energy transfer to endogenous oxygen in cancer cells to enhance X-PDT efficacy. It also features intrinsic NIR emission originated from metal-to-ligand charge transfer (MLCT) to act as an excellent imaging probe. Meanwhile, its large cavity can encapsulate and concentrate low water-soluble molecules for anticancer drug delivery. These multi-functions are implemented and demonstrated by loading coumarin into cage and further micellization with DSPE-PEG2000 into nanoparticles (CMNPs) for efficient subcellular endocytosis and uptake. The cancer treatments in vitro and in vivo show a promising antitumor performance by this self-assembled Os-nanocage, providing a conceptual protocol to combine cage-cargo drug transport with diagnosis and treatment for collaborative cancer theranostics by virtue of multi-functions synergism on a single nanomaterial platform.

A radio- and photosensitizing Os(II)-based nanocage for combined radio/chemo/x-ray induced photodynamic therapies, NIR-imaging and drug delivery

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