The charge-transfer (CT) complexes of a series of 4,4,5,5-tetramethylimidazolin-1-oxyls substituted with 4-(N-alkylpyridinium) groups at the 2-position with two radical anions, tetrafluorotetracyanoquinodimethanide (TCNQF4–) and hexacyanobutadienide (HCBD–) were prepared and their magnetic properties were investigated in the temperature range of 5 to 300 K. Ferromagnetic interaction was observed for the three CT complexes. Furthermore, the magnetic measurement at lower temperatures than 5 K showed that these CT complexes exhibited a ferromagnetic phase transition between 0.4 and 0.55 K. Consequently, the present CT complexes make a group of another type of organic ferromagnets without any magnetic metal elements.