The properties of two coordination polymers formed by the coordination of isonicotinylhydrazine (INH) and 1,3,5-bezenetricarboxylic acid (H3BTC) to Zn2+ or Co2+ ions were studied by a combination of single-crystal X-ray diffraction analysis and density functional calculations. The coordination polymer formed with Co2+ ion, [Co­(INH)­(HBTC)]­(CH3CN)·H2O, named as 1, forms a 2D coordination polymer presenting potential voids in its structure, whereas the coordination polymer formed with Zn2+ ion, [Zn1.5(INH)­(BTC)­(H2O2)]·3H2O, named as 2, forms a 1D ladder-shaped structure. The magnetic study carried out on 1 showed a weak antiferromagnetic coupling, and this property was considered theoretically. Additionally, the electronic properties of 1 were studied by theoretical substitution of Co2+ for Zn2+ to give 1Zn. Compound 2 was also studied by theoretical computational calculations showing quite different electronic properties related to 1. Even composed by different ions, both compounds are semiconductors. The theoretical adsorption of O2 and N2 molecules on 1 and 1Zn was also performed. The results indicated that O2 molecules are better adsorbed in the magnetic compound, highlighting a new important property to be observed on gas adsorption.