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 Abstract CuFeSe2 nanomaterial with high thermal conversion efficiency, well superparamagnetism, effective x-ray attenuation ability, multifunctional groups and excellent biocompatibility is beneficial to the construction of multimodal imaging probes which can combine various imaging modes to provide a synergistic advantage over a single imaging mode. This study aimed to develop a novel multimodal nanocontrast agent CuFeSe2@diethylenetriaminepentaacetic acid (DTPA)-Gd to obtain imaging information with high specificity, high sensitivity and high contrast. The morphology and physical characteristics of CuFeSe2@DTPA-Gd were detected by transmission electron microscope, scanning electron microscope, x-ray single crystal diffraction, vibrating sample magnetometer and fourier transform infrared spectrometer. The toxicity of CuFeSe2@DTPA-Gd in vivowas evaluated by hematoxylin-eosin staining. The imaging capability of CuFeSe2@DTPA-Gd in vitro and in vivowas evaluated by magnetic resonance imaging (MRI) and computed tomography (CT). This study successfully prepared nanoparticles CuFeSe2@DTPA-Gd, and experimental results in this study demonstrated CuFeSe2@DTPA-Gd is expected to be a useful CT and MRI T1-weighted imaging/T2- weighted imaging three-modal contrast agent in clinic.