The synthesis, structural characterization, and excited-state dynamics of series of diketopyrrolopyrrole (DPP) bridged homodinuclear Ir(III) and heterodinuclear Ir(III)/Pt(II) complexes is described. Steady-state and time-resolved photoluminescence along with transient absorption measurements were used to probe the nature of the emissive and long-lived excited states. Upon excitation into the (1)DPP ligand-localized excited state in the presence of coordinated Ir(III) or Pt(II) metal centers, the intersystem crossing is enhanced, leading to a quenching of the (1)DPP fluorescence and the formation of the long-lived (τ ≈ 30-40 μs) (3)DPP excited state in all instances.