The synthesis and characterization of two manganese(II) complexes formally each featuring two cis-tetracyanoethylenide radical anionic ligands (TCNE center dot(/-)) are reported. In each case, tris(pyrazol-1ylmethyl)amine serves as a capping ligand, blocking three facial coordination sites. Crystal structures show that the two TCNE anions in each molecule exhibit an intramolecular stacking interaction that forms what can be considered a coordinated (TCNE2)(2-) moiety. These molecules are presumed to be structural models of some of the local bonding in the family of amorphous, ferrimagnetic, M[TONE](2)center dot y(solvent) coordination polymer magnets. Magnetic measurements indicate that the (TCNE2)(2-) bridge is diamagnetic and not a good mediator of magnetic exchange, a result that might explain the observed lower ordering temperatures in some of the polymer magnets.