Three new complexes [CuL(N3)2] (1), [CuL(SCN)2] (2), and [CoL(SCN)3] (3) (L = 1,4,7-tribenzyl-1,4,7-triazacyclononane) have been synthesized and structurally characterized. Complex 1 crystallizes in monoclinic space group P2(1)/n with unit cell parameters a = 14.105(7), b = 8.999(5), c = 21.603(11) Å, β = 100.470(7)°. While 2 crystallizes in triclinic space group P-1 with unit cell parameters a = 9.6380(16), b = 10.6993(18), c = 15.798(3) Å, α = 106.636(3), γ = 116.478(3)°. Complex 3 crystallizes in trigonal space group P-3c1 with unit cell parameters a = 14.744(3), b = 14.744(3), c = 16.098(4) Å, γ = 120°. Elemental analysis, IR, UV-vis spectra of complexes 1-3 and ESR spectra of complexes 1-2 were also determined.