A series of mononuclear five-coordinate cobalt(II) complexes, [Co(X)(dbdmp)]Y, where dbdmp = N, N-diethyl-N′,N′-bis((3,5-dimethyl-1H-pyrazol-1-yl)methyl)ethane-1,2-diamine, X = N À 3 /NCO − /NCS − and Y = PF À 6 /BF À 4 /ClO À 4 , have been synthesized and characterized by microanalyses and spectroscopic techniques. Crystal structures of [Co(N 3 )(dbdmp)]PF 6 (1), [Co(N 3 )(dbdmp)]ClO 4 (3), [Co (NCO)(dbdmp)]PF 6 (4), [Co(NCO)(dbdmp)]ClO 4 (6), and [Co(NCS)(dbdmp)]ClO 4 (9) have been solved by single-crystal X-ray diffraction studies and showed that all the complexes have distorted trigonal bipyramidal geometry; PF À 6 counter anion containing complexes [Co(N 3 )(dbdmp)]PF 6 and [Co(NCO)(dbdmp)]PF 6 have chiral space groups. The binding ability of synthesized complexes with CT-DNA and bovine serum albumin (BSA) has been studied by spectroscopic methods and viscosity measurements. The experimental results of absorption titration of cobalt(II) complexes with CT-DNA indicate that the complexes have ability to form adducts and they can stabilize the DNA helix. The cobalt(II) complexes exhibit good binding propensity to BSA protein.