Hexacyanobutadiene (HCBD) and M(CO)(x) (M = V, x = 6; Fe, x = 5) react in CH2Cl2 to form new organic-based magnets of M[HCBD](2)center dot z(CH2Cl2) composition. Analysis of the IR spectrum [M = V: v(CN) 2193 and 2116 cm(-1) (fwhh similar to 400 cm(-1)); Fe: 2196 and 2145 (fwhh similar to 150 cm(-1))] suggests that HCBD is reduced to the radical anion, [HCBD](center dot-), and the broadness suggests multiple and variable nitriles sites are coordinated to the V(II), leading to a complex mixture of magnetic couplings and behaviors that deviate from paramagnetic behavior below similar to 150 K, and a frustrated magnet with T-c approximate to 9 K is observed for V[HCBD](2), the first cyanocarbon-based frustrated magnet. Fe[HCBD](2) behaves as a weak ferromagnet (canted antiferromagnet) with some spin glass behavior with a 10 K T-c.