Permanent magnets (PMs) based on manganese show significant potential for applications in electric motors and devices as an alternative to Rare-earth PMs (REPMs). The metastable ferromagnetic τ phase of the Mn-Al system has magnetic performance between the REPM Nd-Fe-B magnets and the lower performance ferrite magnets. However, the maximum performance in Mn-Al PMs has not reached its theoretical limit, in part due to challenges in controlling crystalline defects such as anti-phase boundaries (APBs). APBs act as nucleation sites for domain reversal in Mn-Al and negatively affect magnetization by interrupting the L10 ordering, placing Mn atoms into AFM-coupled Mn-Mn configurations. In this study, Ab-initio modeling was used to screen ternary elements based on their affinity to segregate to the APB and on their preference for FM configuration. The ternary element addition of 1 at.% Ti lowered the density of APBs as observed in a transmission electron microscope. The 1 at.% Ti addition was observed to improve (BH)max over the base alloy, by preserving Hci and improving Mr. It also significantly increased the fraction of twin boundaries in the τ phase. AFM behavior that was observed in the base alloy during TC heating experiments (Néel behavior) and high-field VSM measurements (spin-flop behavior) was effectively suppressed with the addition of Ti. Additionally, the Ti addition thermally stabilized Hci at 550 °C, improving τ phase processability. Other candidate elements, Cr, V, and Zr, were modeled to have similar potential for minimizing APBs when added to Mn-Al.