Readily available, air-stable DCNQIH2 (i.e., 1,4-NC·NH·C6H4·NH·CN) affords, in a very simple manner, crystals of [Mn(DCNQI)(bridge)]2DMF (where bridge = 4,4′-bipyridine or 1,2-bis(4-pyridyl)ethylene) in which there are [(Mn2+)(DCNQI2−)]n sheets held together by 4,4′-bipyridine or 1,2-bis(4-pyridyl)ethylene pillars. This approach via DCNQIH2 promises convenient general entry into new types of DCNQI-based coordination polymers and could lead to new materials with interesting and possibly useful magnetic/electronic properties