We found the giant negative magnetoresistance in the one-dimensional π-dsystem TPP[Fe(Pc)(CN)2]2below 50K. The large negative magnetoresistance was observed for the field along thea-axis, while the small one along thec-axis. We also observed the anisotropic Curie behavior of the magnetic susceptibility. The large (small) magnetoresistance was observed in the field orientation for the large (small) magnetic susceptibility. The reduction of the spin-flip scattering of the itinerant electrons by the local moments under the magnetic field was proposed as the origin of the negative magnetoresistance. In the isostructural compound TPP[Co(Pc)(CN)2]2we observed the large positive magnetoresistance. This positive magnetoresistance cannot be explained in terms of the orbital effects under the field.