The crystal structures of [MnTPP]{Ni[S2C2H(CN)](2)} [MnTPP = (meso-tetraphenylporphinato)manganese(lll)] and [MnTPP]{Ni[S2C2(CN)(2)](2)} have been determined. These salts possess trans-mu-coordination of S = 1/2 {Ni[S2C2H(CN)](2)}center dot(-) and {Ni[S2C2(CN)(2)](2)}center dot(-) to Mn(lll) and form parallel 1-D coordination polymer chains exhibiting (CN)-C-nu at 2210 and 2200 and 2220 and 2212 cm(-1), respectively. The bis(dithiolato) monoanions are planar and bridge two cations with MnN distances of 2.339(16), and 2.394(3) angstrom, respectively, which are comparable to related MnN distances observed for [MnTPP][TCNE]-x(solvates). In addition, [MnTP'P]{Ni[S2C2(CN)(2)](2)} {H2TP'P = mesotetrakis[3,5-di-tert-butyl-4-hydroxyphenyl)porphyrin] and [MnTP'P(OH2)]{Ni[S2C2(CN)(2)](2)} were prepared. The latter forms isolated paramagnetic ions. The room-temperature values of chi T for 1-D [MnTPP]{Ni[S2C2H(CN)](2)}, [MnTPP]{Ni[S2C2(CN)(2)](2)}, and [MnTP'P]{Ni[S2C2(CN)(2)](2)} are 2.55, 3.28, and 2.86 emu K/mol, respectively. Susceptibility (chi) measurements between 2 and 300 K reveal weak antiferromagnetic interactions with Theta = -5.9 and -0.2 K for [MnTPP]{Ni[S2C2H(CN)](2)} and [MnTPP]{Ni[S2C2(CN)(2)](2)}, respectively, and stronger antiferromagnetic coupling of -50 K for [MnTP'P]{Ni[S2C2(CN)(2)](2)} from fits of chi(T) to the Curie-Weiss law. The 1-D intrachain coupling, J(intra), of [MnTPP]{Ni[S2C2H(CN)](2)} and [MnTPP]{Ni[S2C2(CN)(2)](2)} was determined from modeling chi T(T) by the Seiden expression (H = -2JS(i)-S-j) with J/k(B) = -8.00 K (-5.55 cm(-1); -0.65 meV) for [MnTPP]{Ni[S2C2H(CN)](2)}, J/k(B) = -3.00 K (-2.08 cm(-1); -0.25 meV) for [MnTP'P]{Ni[S2C2(CN)(2)](2)}, and J/k(B) = -122 K (-85 cm(-1)) for [MnTP'P]{Ni[S2C2(CN)(2)](2)}. These observed negative J(intra)/k(B) values are indicative of antiferromagnetic coupling. These materials order as ferrimagnets at 5.5, 2.3, and 8.0 K, for [MnTPP]{Ni[S2C2H(CN)](2)}, [MnTPP]{Ni[S2C2(CN)(2)](2)}, and [MnTP'P]{Ni[S2C2(CN)(2)](2)}, respectively, based upon the temperature at which maximum in the 10 Hz chi'(T) data occurs. [MnTP'P]{Ni[S2C2(CN)(2)](2)} has a coercivity of 17 700 Oe and remanent magnetizations of 7250 emu Oe/mol at 2 K and 17 Oe and 850 emu Oe/mol at 5 K; hence, upon cooling it goes from being a soft magnet to being a very hard magnet.