Metal–organic frameworks (MOFs), such as the magnetic resonance imaging-fit MIL-100 based on Fe, are gaining significant attention as versatile theranostics with high-loading capability. Moreover, as MOFs can be engineered to target tumors, there is much interest in applying them for precise pin-point treatment of cancer. Herein, Pd nanoparticles within MIL-100(Fe) are generated to create MOFs with remarkable photothermal conversion properties for cancer therapy. The Pd-loaded MIL-100(Fe) (Pd@MIL-100(Fe)) are stabilized with biocompatible block copolymers to generate MOFs with PEGylated surfaces. This is achieved by directly mixing poly(ethylene glycol)-poly(L-aspartic acid) (PEG-p(Asp)) or dopamine-modified PEG-p(Asp) (PEG-p(Asp-Dopa)) block copolymers with the MOFs in aqueous conditions. The resulting block copolymer-stabilized MOF hybrids are stable in physiological conditions. Particularly, the Pd@MIL-100(Fe)/PEG-p(Asp-Dopa) hybrids show enhanced blood circulation and increased accumulation in B16F10 melanoma. Furthermore, when irradiated with 808 nm light, the Pd@MIL-100(Fe)/PEG-p(Asp-Dopa) hybrids rapidly increase the temperature to 50 °C, enabling tumor remission. The surface-stabilized Pd@MIL-100(Fe)/polymer hybrids open viable opportunities for innovating MOF/polymer hybrid-based approaches for drug delivery.
