The hydrothermal reactions of CuBr2, CuBr, and 2,2'-dipyridyl have resulted in the synthesis of three new compounds. Cu3Br4(C10H8N2)(2) (1) is a molecular phase; CuBr2(C10H8N2) (2) is a one-dimensional chain structure; and [Cu-2(OH)(2)(C10H8N2)(2)][Cu4Br6] (3) crystallizes in a two-dimensional sheet structure. All three compounds were characterized by single-crystal X-ray diffraction. Crystal data for 1, triclinic, space group P (1) over bar (No. 2) with a = 10.604(2) Angstrom, b = 11.642(2) Angstrom, c = 11.688(2) Angstrom, alpha = 61.965(5)degrees, beta = 68.965(5)degrees, gamma = 69.523(5)degrees, Z = 2; 2, monoclinic, space group C2/c (No. 15) with a = 16.766(4) Angstrom, b = 9.287(2) Angstrom, c = 7.392(2) Angstrom, beta = 110.536(6)degrees, Z = 4; 3, monoclinic, space group P2(1)/n (No. 14) with a = 10.907(3) Angstrom, b = 6.0677(13) Angstrom, c = 21.620(5) Angstrom, beta = 90.542(4)degrees, Z = 4.