A C–H bond activation strategy based on electrochemical activation of a metal hydride is introduced. Electrochemical oxidation of ( tBu 4 PCP)IrH 4 ( tBu 4 PCP is [1,3-( t Bu 2PCH 2)-C 6H 3] –) in the presence of pyridine derivatives generates cationic Ir hydride complexes of the type [( tBu 4 PCP)IrH(L)] + (where L = pyridine, 2,6-lutidine, or 2-phenylpyridine). Facile deprotonation of [( tBu 4 PCP)IrH(2,6-lutidine)] + with the phosphazene base tert-butylimino-tris(pyrrolidino)phosphorane, t BuP 1(pyrr), results in selective C–H activation of 1,2-difluorobenzene (1,2-DFB) solvent to generate ( tBu 4 PCP)Ir(H)(2,3-C 6F 2H 3). The overall electrochemical C–H activation reaction proceeds at room temperature without need for chemical activation by a sacrificial alkene hydrogen acceptor. This rare example of undirected electrochemical C–H activation holds promise for the development of future catalytic processes.