The larch-fruit-like acetylferrocene micro-nanomaterials and beltlike acetylferrocene micro-nanomaterials have been cross-correspondingly prepared in bidirection by the top-down and bottom-up approach, respectively, and characterized by scanning electron microscope, transmission electron microscope and X-ray diffractometer. UV-Vis absorption spectra show that the redshift was found in the acetylferrocene micro-nanomaterials compared to that in solution. The formation mechanism of the acetylferrocene micro-nanomaterials is also proposed. This work provides a new strategy for the material synthesis and preparation and may realize the reuse of organometallic materials.