We investigate the magnetic and electronic properties of Co films on Fe3O4(001) achieved through epitaxial growth using magnetron sputtering. X-ray magnetic circularly dichroism measurements characterize the atomic magnetism. Compared to Co films on the MgO substrate, Co on Fe3O4 exhibits a 96% enhancement in orbital magnetic moment (from 0.25 to 0.49 µB/atom) and an increase in spin magnetic moment (from 1.37 to 1.53 µB/atom), resulting in an increased mratio(ml/ms) from 0.18 to 0.32. This enhancement of the orbital moment emerges as a consequence of the interface interaction between Co and Fe3O4. Density functional theory calculations attribute this heightened orbital magnetic moment to the robust electronic exchange interactions. Our findings not only offer insights into the modulation of magnetic and electronic characteristics in Co-based magnetic heterostructures but also provide valuable implications for the potential application of magnetic oxide/ferromagnetic heterostructures in future spintronic devices.