Recently, we reported an antiferromagnetic ground state for equiatomic Al-Cr in the B2 structure. Here, by a joint theoretical–experimental study, we investigate the effect of Co additions to the Al-Cr alloy with the aim to synthesize a ferromagnetic B2 phase. Al50Cr38Co12 (at.%) is prepared by arc melting from high-purity raw materials and solidifies into a combination of a Co-enriched B2 phase, a Co-depleted BCC phase, and an Al8Cr5 intermetallic phase. The as-cast alloy is ferromagnetic with a Curie point of 260 K, primarily due to the presence of about 54% B2 phase. Subsequent annealing decreases the fraction of the B2 phase to 27% with depletion of Cr from 20.2 at.% to 16.1 at.%, which leads to a reduction in its ferromagnetic behavior. Calculations based on Density Functional Theory (DFT) predict a corresponding decrease in the total magnetic moment and Curie temperature of the B2 phase by annealing. The present findings highlight the roles of Cr and Co in facilitating the formation of a metastable ferromagnetic B2 phase in this alloy.