By using the short-time electrocrystallization technique, phthalocyanine (Pc)-based Mott insulator Co(Pc)(CN)2 . 2CHCl3 nanocrystals were fabricated and applied to organic light-emiting diodes (OLEDs). The fabricated device having the configuration ITO/Co(Pc)(CN)2 . 2CHCl3/Alq3/Al, in which ITO is indium-tin oxide and Alq3 is tris(8-hydroxyquinolinato)aluminum, showed clear emission from Alq3, suggesting the Mott insulator Co(Pc)(CN)2 . 2CHCl3 can work as useful hole-injection and transport material in OLEDs.