In this research, a Ni-Fe mold insert for the efficient replication of high aspect-ratio microstructure arrays was fabricated via hard X-ray lithography and an electroforming process. For the X-ray exposure on a photoresist, a gold-based X-ray mask was prepared with conventional UV photolithography. The gold thickness was designed to be over 15 μm to prevent development underneath the absorber and to enhance the adhesion strength between the photoresist and substrate. By using the X-ray mask, a positive-type photoresist was selectively exposed to X-ray under an exposure energy of 4 kJ/cm3. Thereafter, the exposed region was developed in a downward direction to effectively remove the residual photoresist from the substrate. During the evaporation process, deionized water mixed with a surface additive prevented the bending and clustering of the photoresist microstructure arrays by lowering the capillary force, resulting in a defect-free mother structure for electroforming. Lastly, the mother structure was uniformly Ni-Fe electroformed on a conductive substrate without the formation of any pores or detachment from the substrate. Based on the proposed microfabrication process, a Ni-Fe mold insert with a 183 μm pattern size, 68 μm gap size, 550 μm height, 2116 microcavities and a hardness of 585 Hv was precisely manufactured. It can be utilized for the mass production of high aspect ratio metal and ceramic microstructure arrays in micro molding technologies.