One of the barriers for wide usage of hydrogen energy system is efficient storage. To store more hydrogen efficiently, physisorption is a choice among the others with high storage performance, reversibility, and lifecycles. Metal organic framework (MOF) structured organometallic orotate-Co(II) complexes could serve as sorbents which store hydrogen by physisorption. In this work, mono- and bidentate MOF structured orotate-Co(II) complexes are synthesized, characterized, and then investigated for hydrogen storage experimentally and theoretically. It is found that these compounds could store hydrogen. Especially, the monodentate complex could uptake hydrogen better than the other. Storage performances for mono- and bidentate complexes were 0.80 and 1.15 wt% at 77 K and approximately 80 bars experimentally, 1.03 and 1.16 wt% theoretically for the same conditions.