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The morphology evolution of zinc continuous electrodeposits with nano-sized crystals on the ferrite substrate has been studied by in-situ scanning tunnel spectroscopy (STM). It is found that the morphology of zinc electrodeposits varies from initial granules with a size of about 30 nm to layered platelets with increasing deposition time. Meanwhile, the crystal structure of the zinc electrodeposits is identified to be hexagonal η-phase by X-ray diffraction. The orientation relationship between zinc crystals and the substrate surface can be interpreted in terms of the misfit and the atomic correspondence of the interphase boundary between the η-phase deposits and α-Fe substrate.