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Nanodiamonds with magnetic resonance imaging (MRI) and targeted drug delivery to exert combined effects for biomedical applications have been considered to be an urgent challenge. Herein, a novel bio-nanoarchitectonics (Fe[sub.3]O[sub.4]@NDs) with simultaneous imaging and therapeutic capacities was fabricated by covalently conjugating nanodiamonds (NDs) with Fe[sub.3]O[sub.4]. Fe[sub.3]O[sub.4]@NDs exhibited better biocompatibility and excellent photothermal stability with superb photothermal conversion performance (37.2%). Fe[sub.3]O[sub.4]@NDs has high doxorubicin (DOX) loading capacity (193 mg/g) with pH and NIR-responsive release characteristics. Fe[sub.3]O[sub.4]@NDs loading DOX showed a combined chemo-photothermal inhibitory effect on the tumor cells. Enhanced T[sub.2]-weighted MRI contrast toward the tumor, with the assistance of a magnetic field, convinced the Fe[sub.3]O[sub.4]@NDs gathered in the tumor more efficiently and could be used for MRI-based cancer diagnosis. Our results revealed an effective strategy to achieve a stimuli-sensitive nanoplatform for multifunctional theranostics by the combined action.