The attractive electronic properties of metal-pyrazine materials�electrical conductivity, magnetic order, and strong magnetic coupling�can be tuned in a wide range depending on the metal employed, as well as its ligand-imposed redox environment. Using solvent-directed synthesis to control the dimensionality of such systems, a discrete tetranuclear chromium(III) complex, exhibiting a rare example of bridging radical pyrazine, has been prepared from chromium(II) triflate and neutral pyrazine. The strong antiferromagnetic interaction between Cr III (S = 3/2) and radical pyrazine (S = 1/2) spins, theoretically estimated at about −932 K, leads to a thermally isolated S T = 4 ground state, which remains the only populated state observable even at room temperature.