An improved performance of organic light-emitting diodes has been obtained by using 4-(dicyanomethylene)-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4Hpyran (DCJTB) as an ultrathin emitting layer. When 0.1nm DCJTBwas inserted between the hole-transporting layer and electron-transporting layer, for an unoptimized device indiumtin oxide (ITO)/naphtylphenyliphenyl diamine (NPB)/DCJTB (0.1nm)/8-hydroxyquinoline aluminum (Alq3)/Al, the maximum brightness was 1531 cdm−2 at 15V. Compared with doped devices ITO/NPB/Alq3:DCJTB (1%)/Alq3/LiF/Al, a higher efficiency has been achieved. Compared with the conventional device ITO/NPB/Alq3/Al, the inserted device has a slightly higher current efficiency and lower turn-on voltage. We suggest the ultrathin DCJTB layer acts as trap for carriers, and the accumulated holes at the hole-transport layer/electron-transport layer interface have enhanced the electric field in the electron-transport layer and improved the electron injection at the cathode.