The donor (D)/acceptor (A) assembly reaction of the paddlewheel-type diruthenium(II,II) complex [Ru-2(2,4,6-F3PhCO2)(4)(THF)(2)] (2,4,6-F3PhCO2- = 2,4,6-trifluorobenzoate; abbreviated hereafter as [Ru-2]) with 7,7,8,8-tetracyano-p-quinodimethane (TCNQ) in a p-xylene/CH2Cl2 solvent system led to the formation of a two-dimensional layered compound, [{Ru-2(2,4,6-F3PhCO2)(4)}(2)(TCNQ)]center dot 2(p-xylene)center dot 2CH(2)Cl(2) (1). As expected from this D/A combination, 1 has a one-electrontransfer ionic state with the D(2)(0.5+)A(-) formulation. This state formally derives a heterospin state composed of S = 1 for [Ru-2(II,II)], S = 3/2 for [Ru-2(II,III)], and S = 1/2 for TCNQ(center dot-), possibly causing intralayer ferrimagnetic spin ordering. Most of these types of compounds have an antiferromagnetic ground state because of the coupling of ferrimagnetically ordered layers in dipole antiferromagnetic interactions. However, 1 became a three-dimensional ferrimagnet with T-C = 91 K because of the presence of interlayer ferromagnetic interactions.