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In this study, we report the synthesis and application of the novel cyclometallated luminescent Ir(III) complex 1 bearing the C^C^C ligand as a probe and inhibitor of Aβ fibrillation. We envisage that this kinetically-inert Ir(III) complex may be potentially developed as a dual-purpose probe and inhibitor of Aβ aggregation for Alzheimer’s disease diagnosis and treatment.