The syntheses, crystal structures, and powder magnetic studies of several new quasi-planar bibridged CunX2n+22õ ligomers (n = 3, 4, 6, and 7; X = Cl or Br) are reported, based on the 1 -methylpyridinium (CftHsN'U and 1,2-dimethylpyridinium (C7H|0N)+ cations. These include (C7HioN)2Cu3Br8, (C6H8N)2Cu4C1io, (C7H|0N)2Cu6-Clu, and (C7H|0N)2Cu7Bri6. Crystallographic data: (C7HioN)2Cu3Br8, triclinic, space group PI, a = 7.947(2) A,b = 8.799(2) A, c = 9.840(2) A, a = 86.95(2)°, = 76.23(2)°, y = 71.54(2)°, V = 633.6(3) A3, Z=2,dx = 2.78 g/cm3, and R = 0.0483; (CeHgN^CmClio, monoclinic, space group P2\!n, a = 11.759(2) A, b = 9.056(2)A, c = 12.048(3) k,J = 106.21(2)°, V = 1232.1(5) A3, Z = 2, dx = 2.15 g/cm3, and 7? = 0.0321; (C7HI0N)2-Cu6Cl|4, triclinic, PI, a = 8.997(3) A, b = 9.288(3) A, c = 11.540(4)A, a = 80.53(2)°, /? = 67.82(2)°, y = 60.22(2)°, V = 714.7(4) A3, Z = 1, dx = 2.34 g/cm3, and R = 0.0363; (C6H8N)2Cu7Bri6, triclinic, PI, a = 7.237(2) k,b= 10.880(2) A, c = 12.880(2) A, a = 89.47(2)°, /? = 75.08(2)°, y = 79.48(2)°, V = 962.7(3) A3, Z = 1, dx = 3.35 g/cm3, and R = 0.0520.A common feature of the structures is the existence of oligomers containing quasi-planar symmetric bibridged finite chains of edge-sharing CuXa (X = halide) monomeric units.The n = 3 oligomers aggregate into chains through the formation of asymmetric bibridged linkages between terminal copper ions on adjacent trimers. In the n = 4 salt, the oligomers aggregate into stacks in which pairs of the copper ions extend their coordination sphere by forming a long, semicoordinate bond to a halide ion from a neighboring oligomer. For both the n = 3 and n = 4 salts, the pyridinium cations lie parallel to and directly above and below the anionic oligomers, separating the chains. In the n = 6 and n = 7 salts, the stacks formed in this manner interdigitate, forming two-dimensional slabs. The slabs are separated by the organic cations. The magnetic properties of compounds are dominated by antiferromagnetic intraoligomer interactions. Thus, the n = 4 and n = 6 salts depopulate into singlet ground states at low temperature. In contrast, the n = 3 and n -7oligomers have S = '/2 ground states. Expressions for the magnetic susceptibility of the n = 6 and n = 1 oligomers were obtained by diagonalization of a nearest neighbor Heisenberg Hamiltonian. The data were fit to these expressions, with inclusion of a mean field correction for interoligomer exchange. The intra-oligomer exchange coupling constants are