Ordered hard magnetic L10-FeNi has attracted attention as a candidate for rare-earth-free permanent magnet with a large maximum magnetic energy product. Fabricating L10-FeNi is a big challenge using conventional methods due to its low order-disorder transition temperature, 320 °C. In this work, high-quality ordered L10-FeNi films were fabricated by using molecular beam epitaxy directly on Al2O3 (0001) substrate with a two-step co-deposition method below 250 °C. The films were epitaxially grown with [111] orientation, confirmed by reflection high energy electron diffraction and x-ray diffraction patterns. An order-disorder phase transition at 320 °C was observed in temperature dependent electrical resistivity curve. The two-step molecular beam epitaxy grown film exhibited high uniaxial magnetic anisotropy constant, Ku, up to 1.15 × 106 J/m3. The obtained Ku value is comparable to previous result for FeNi along [100] growth direction, indicating an isotropic Ku. This work provides an effective molecular beam epitaxy growth method of high-quality ordered L10-FeNi (111) film for the development of the next-generation rare-earth-free permanent magnet.