In this paper, a novel approach to obtain a ferromagnetic material for smart applications was implied. A combination of mechanical alloying (MA) and plasma spheroidization (PS) was applied to produce Ni₃₆ Al₂₇ Co₃₇ spherical powder. Then its structure was systematically studied. It was shown that homogenization of the structure occurs due to mechanism of layered structure formation. The dependence of the lamella thickness on the energy dose input at MA was defined. It was found that 14.7 W·h/g is sufficient to obtain lamella thickness of 1 µm and less. The low-energy mode of a planetary mill with rotation speeds of the main disk/bowl of 150/−300 rpm makes it possible to achieve a uniform element distribution upon a minimal amount of impurity. During MA in an attritor Ni₃ Al-type intermetallic compounds are formed that result in more intensive degradation in particle size. Plasma spheroidization of the powder after MA allowed obtaining Ni₃₆ Al₂₇ Co₃₇ spherical powder. The powder had a fine β + γ-structure. The particle size distribution remains almost unchanged compared to the MA stage. Coercivity of the powder is 79 Oe. The powder obtained meets the requirements of selective laser melting technology, but also can be utilized as a functional filler in various magnetic composites.