We have studied the magnetotransport properties of La0.67−xBixSr0.33MnO3 (x = 0, 0.3, 0.4, 0.5). The x ≤ 0.3 samples show metal–insulator transitions, whereas x ≥ 0.4 samples exhibit an insulating behaviour at zero field. Notably, two low‐temperature upturns were observed for La0.37Bi0.3Sr0.33MnO3, which indicates the existence of two different mechanisms. La0.27Bi0.4Sr0.33MnO3 shows field‐induced metallic behavior due to the melting of charge ordering with applied magnetic field. A large magnetoresistance of ∼100% is observed for La0.27Bi0.4Sr0.33MnO3 at ∼90 K. On the other hand, La0.37Bi0.3Sr0.33MnO3 exhibits a nearly constant large magnetoresistance of ∼80% between ∼30 and 250 K, which decreases outside this temperature range. The observed anomalous low‐temperature magnetotransport properties of La0.67−xBixSr0.33MnO3 are shown to arise from the coexisting phases of ferromagnetic metallic and antiferromagnetic charge‐ordered insulating states.