The　combination　of　non-invasive　fluorescence　(FL)　and　magnetic　resonance　(MR)　imaging　can　compensate　for　disadvantages　in　terms　of　resolution　and　sensitivity.　However,　the　preparation　of　dual-mode　probes　simultaneously　exhibiting　strong　brightness　and　high　MR　response　is　challenging.　A　multifunctional　nanoprobe　was　synthesized　for　targeted　photoluminescence　(PL)　and　MR　dual-modal　imaging.　It　was　obtained　by　conjugating　iridium(III)　complexes,　gadolinium(III)　and　the　peptide　arginine-glycine-aspartate　(RGD)　onto　silica　nanoparticles　(Ir@SiO2-Gd-RGD　NPs).　They　are　highly　water　soluble,　have　an　average　diameter　of　similar　to　50　nm,　and　emit　strong　yellowish　green　PL　(with　excitation/emission　peaks　at　380/572　nm).　Simultaneously,　the　nanoprobes　exhibit　high　MR　response　with　a　longitudinal　relaxation　of　7.16　mM(-1)　s(-1).　Instead　of　simple　encapsulation,　Ir　(III)　complexes　were　covalently　conjugated　to　silica　matrix　to　enhance　the　chemical　and　photochemical　stability　of　the　nanoprobes.　The　excellent　biocompatibility　and　PL/MR　dual　modal　imaging　capability　of　the　NPs　is　demonstrated　using　HeLa　cells　and　mice　as　models.