As eries of dppnc-and neocuproine-based Cu I complexes (dppnc = 7,8-bis(diphenylphosphino)-7,8-dicarbanido-undecaborate) are synthesized and the emission color of these Cu I complexes can be tuned from green to deep red via rational modification of the neocuproine ligand structure. The molecular structures of the emissive Cu I complexes, Cu(dppnc)-G (green emitting), Cu(dppnc)-Y (yellow emitting),a nd Cu(dppnc)-R( red emitting), are characterized and their electronic structures and related transition properties are elucidated by photo-physical and computational (density functional theory) studies. The calculation results suggest that thermally activated delayed fluorescence (TADF) is the emission mechanism for these Cu I complexes. Efficient solution-processedg reen-,y ellow-, and red-emitting OLEDs are fabricated based on the emissive complexes as the dopants. High external quantum efficiency (EQE) of 15.20 %a nd current efficiencyo f4 8.15 cd A À1 at 1000 cd m
À2are achieved in the green-emitting device with Cu(dppnc)-G. Am aximum EQE of 10.17 %, CIE coordinates of (0.61, 0.38) and am aximum electroluminescent peak of 631 nm are achieved in the red device based on Cu(dppnc)-R.