This study describes the biological and anticancer properties of followed coordination compounds. IR spectra, magnetic properties, thermal analyses and crystal structures of six cyanido-complexes derivatives with [M II (CN) 4 ] 2- (M II = Ni and Pd) and [Co(CN) 6 ] 3- anions and N - bishydeten ( N,N -bis(2-hydroxyethyl)ethylenediamine) as a capping ligand have been previously reported. Here, we investigated these complexes denoted as[Ni( N-bishydeten )Ni(CN) 4 ] ( C1 ), [Zn 2 ( N-bishydeten ) 2 Ni(CN) 4 ] ( C2 ), [Ni( N-bishydeten )Pd(CN) 4 ] ( C3 ), [Cd( N-bishydeten ) 2 ][Pd(CN) 4 ] ( C4 ), [Ni 2 ( N-bishydeten ) 2 Co(CN) 6 ].3H 2 O ( C5 ) and K[Cd( N-bishydeten )Co(CN) 6 ].1.5H 2 O ( C6 ), which were tested for their anti-proliferative activity against human cervical cancer (HeLa), human colon cancer (HT29), rat glioma (C6) and African green monkey kidney (Vero) cell lines. The DNA/BSA binding affinities of these compounds were also elucidated by spectroscopic titrations, displacement experiments and electrophoresis measurements. Studies on cancerous cells revealed that C1 , C2 , C4 and C6 exhibited significant antitumor activity and inhibited tumor progression in testing cell lines and showed high solubility in the solvent. Absorbance and emission spectra data results revealed that the complexes interact with the DNA via groove binding mode of interaction. Overall, these compounds have been found to demonstrate effective anti-proliferative activity against the cancer cell lines, indicating that they are a potent candidate for preclinical or clinical study.