2,2'',5,5''-Tetrakis(dimethylamino)-p- and m-terphenyls (1 and 2), in which two N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD) moieties are linked through p- and m-phenylene units, respectively, were synthesized, and their CT complexes with TCNQF4 were prepared. In the complexes, 1 and 2 possess two S=112 spins per molecule. The intramolecular interaction between the spins of the two TMPD moieties was found to be antiferromagnetic (2J/k=-42 K) in 1, and ferromagnetic (2J/k=240 K) in 2.