A chemical vapor deposition method has been developed for the synthesis of both Co[TCNE]2 thin-films and VxCo 1-x[TCNE]2 thin-films. Both materials have been previously synthesized by various solution methods. The Co[TCNE] 2 thin-films were characterized by infrared spectroscopy and magnetometer, and were determined to be identical in structure and magnetic behavior to the analogous solution-prepared samples.;VxCo1-x[TCNE] 2, when prepared from solution, showed a composition dependence of the magnetic properties as well as the infrared characteristics. Higher cobalt concentrations led to higher coercive fields with respect to V[TCNE] 2, which has a coercive field of ∼7 Oe at 5 K. At a composition of V0.3Co0.7[TCNE]2 the coercive field is ∼270 Oe at 5 K. The thin-films of this material showed the same infrared characteristics, based on composition, as the solution-prepared compounds. There was, however, no increase in coercive field at any composition, with a maximum coercive field measured as 10 Oe for a composition of V0.45Co0.55[TCNE] 2. |