The preparation, X-ray crystal structures, and magnetic properties of two new isostructural charge transfer salts, (BDH-TTP)M(isoq)(2)(NCS)(4) (M = Cr-III (1), Fe-III (2), BDH-TTP = 2,5-bis(1,3-dithiolan-2-ylidene)-1,3,4,6-tetrathiapentalene, isoq isoquinoline), are reported. Crystal data for 1: monoclinic, space group C2/c (#15), a = 16.1363(9) Angstrom, b = 19.0874(12) Angstrom, c = 12.5075(6) Angstrom, beta = 95.70(4)degrees, V = 3833.2(4) Angstrom(3), Z = 4, R = 0.0516 for 2844 reflections with I > 2sigma(I); for 2: monoclinic, C2/c (#15), a = 16.1938(8) Angstrom, b = 19.1117(11) Angstrom, c = 12.5100(10) Angstrom, beta = 94.265(3)degrees, V = 3861.0(4) Angstrom(3), Z = 4, R = 0.0479 for 2969 reflections with I > 2sigma(I). The crystal structure consists of zigzag mixed organic and inorganic layers, and each layer is formed by mixed columns of BDH-TTP radical cations and paramagnetic metal complex anions. Short intermolecular atomic contacts between donor and anion are observed within the column in the c-direction. The two compounds have weak room-temperature electrical conductivities. ESR measurements show a single signal without separating the donor and anion spins, suggesting a pi interaction between the d and pi electrons. For both compounds ferrimagnetic interactions are observed between the nonequivalent donor and anion spins. These materials exhibit bulk canted weak ferromagnetism below 7.6 K for both 1 and 2.