The ordered body‐centered tetragonal intermetallic phase of FeNi is a promising candidate for high‐performance permanent magnets without rare‐earth elements. However, on earth FeNi is found naturally only in the disordered face‐centered‐cubic A1 phase. Herein, the atomic migration and ordering processes in binary intermetallic phases are investigated within the framework of density‐functional theory. The main objectives are 1) to develop a thorough understanding of the thermally activated diffusion processes at the atomic scale and 2) to make a critical assessment in how far electric field and current effects can be effective means for an enhanced hardening‐by‐ordering of disordered, soft‐ferromagnetic alloys. The scope is extended from FeNi to the hard‐ferromagnetic phases of FePt, FePd, MnAl, and MnGa as well as ternary Fe(Pt,Ni) alloys. These materials cover a wide range of thermal‐ordering time scales and related experimental feasibility.