One of the most significant challenges in the diagnosis of brain cancer is efficient in vivo imaging using nontoxic nanoprobes. Core-shell gold nanorod@MIL-88(Fe) nanostars are successfully constructed as triple-modality imaging (computed tomography/magnetic-resonance imaging/photoacoustic imaging) nanoprobes that show low cytotoxicity, high contrast, high penetration depth, and high spatial resolution for accurate and noninvasive imaging and diagnosis of gliomas.