Porous coordination polymers [Fe2MO(Piv)6(L)x ]n (L is tris(4-pyridyl)pyridine, M = Ni (I) and Co (II); L is tris(4-pyridyl)triazine, M = Ni (III) and Co (IV); x varies from 0.7 to 1.17) are obtained. The structure of polymer I is determined by X-ray diffraction analysis. The choice of the solvent (chloroform or dimethylformamide (DMF)) for the preparation of polycrystalline samples affects the morphology of the crystals. It is found for the studied samples that an increase in the average crystal size (from 1 to 20 μm) and the enhancement of the crystallinity of the samples increase the sorption capacity with respect to hydrogen from 0.7 to 0.9% (78 K, 1 atm).