Solid solutions of VxCo1-x[TCNE](2) composition have been prepared from the reaction of V(CO)(6) and Co-2(CO)(8) in dichloromethane All magnetically order above 280 K for x>0.05 and their coercivity increases with decreasing x, reaching a maximum of 270 Oe for x=0.3 (see Figure). Hence, the magnetic properties of this magnet can be finely tuned via a synthetic organic chemistry methodology.