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Heteronuclear MRI offers broad potential for specific detection and quantification of molecularly targeted agents in diagnosis and therapy planning or monitoring. Here we report a novel method for simultaneous acquisition of dual-nuclei hyper-CEST 129 Xe and 19 F tumor targeting MRI. 129 Xe hyper-CEST MRI, 19 F MRI and fluorescent imaging were integrated into PFOB nanoemulsion as a imaging system for sensitive and selective tumor cells detection. As the complement to 1 H MRI, 129 Xe and 19 F signals can also provide efficient and precise anatomical localization of tumors.