The synthesis, spectroscopic, and magnetic characterization of two new copper(II) and cobalt(II) complexes are described. Both two compounds have the general formula [M(L) 2 (Cl) 2 ], in which <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" id="M1"><mml:mrow><mml:mtext>L</mml:mtext><mml:mo>=</mml:mo></mml:mrow></mml:math> 2-amino-5-bromopyridine. These complexes were prepared in one-step synthesis and characterized by elemental analysis, FTIR, UV-Vis, and EPR spectroscopy. Moreover, the single crystal structure of complex ( 1 ) was studied by the X-ray diffraction method. This compound consists of mononuclear units consisting of two ligands linked to metal via the nitrogen of pyridine ring. The UV-Vis spectra of copper(II) and cobalt(II) complexes show three and five absorption bands, respectively, attributed to the d-d transition of the metal ion, ligand → metal charge transfer, and <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" id="M2"><mml:mi>π</mml:mi><mml:mo>→</mml:mo><mml:msup><mml:mi>π</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:math> or <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" id="M3"><mml:mi>n</mml:mi><mml:mo>→</mml:mo><mml:msup><mml:mi>π</mml:mi><mml:mo>∗</mml:mo></mml:msup></mml:math> transitions of the ligand. The FTIR spectra show MN 2 Cl 2 vibrations at 500–300 <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" id="M4"><mml:mrow><mml:msup><mml:mtext>cm</mml:mtext><mml:mrow><mml:mo>−</mml:mo><mml:mtext>1</mml:mtext></mml:mrow></mml:msup></mml:mrow></mml:math>. The complexes show room temperature magnetic moments of 1.78 BM and 4.12 BM for Cu(II) and Co(II), respectively. The X-band electron spin resonance (ESR) spectra of Cu(II) complex in DMF or DMSO frozen at liquid nitrogen temperature show the typical <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" id="M5"><mml:mi mathvariant="normal">Δ</mml:mi><mml:msub><mml:mi>M</mml:mi><mml:mtext>S</mml:mtext></mml:msub><mml:mo>=</mml:mo><mml:mo>±</mml:mo><mml:mn>1</mml:mn></mml:math> transition.