| Summary: | Process parameters leading to magnetic polymer composites, an essential ingredient in the additive manufacturing of rare-earth-free magnets, are investigated. The induction melting of manganese (Mn) and aluminum (Al), and subsequent annealing at 450, 500, or 550 °C for 20 min, gave rise to ferromagnetic τ–MnAl phase, as well as other phases. The nonmagnetic Al<sub>4</sub>C<sub>3</sub> and oxide phases were then removed by the magnetic separation. Magnetic powders from the magnetic separation were incorporated in polylactic acid (PLA) matrix via a solution route. The remanent magnetization as high as 4.3 emu/g in the powder form was reduced to 2.3–2.6 emu/g in the composites. The reduction in coercivity was minimal, and the largest value of 814 Oe was obtained when the powder annealed at 450 °C was loaded in the composite. The phase composition and hence magnetic properties were even more sensitive to the carbon (C) doping. Interestingly, the addition of 3% C led to coercivity as high as 1445 Oe in MnAl–C powders without further annealing. The enhanced coercivity was attributed to the domain wall pinning by the AlMn<sub>3</sub>C phase, and magnetizations are likely increased by this phase.
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