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The effect of applying a magnetic field during the crystallization process of mechanically milled SmCo9.5 and Sm(Co0.88Fe0.12)9.5 alloys on the nanostructure, exchange coupling, and magnetic properties has been studied. Compared with samples annealed without the magnetic field, there was a noticeable improvement in the intrinsic coercivity iHc, the remanence Br, and the maximum magnetic energy product (BH)max for SmCo9.5 and Sm(Co0.88Fe0.12)9.5 alloys annealed in a 10 kOe field. An improvement of 31.5% of (BH)max was obtained for SmCo9.5 alloy after the magnetic annealing. Better rectangularity of the demagnetization curves was also observed for SmCo9.5 and Sm(Co0.88Fe0.12)9.5 alloys after the magnetic annealing. The improvement in the magnetic properties after magnetic annealing is considered to be the result of enhanced exchange coupling, resulting from modifications of nanostructure induced by the magnetic field during the crystallization process of the mechanically milled alloys in a nearly perfect amorphous state.