A raw hydrogen mixture frequently results in a reduction in conversion efficiency and the generation of undesired by‐products. The application of advanced membrane technology has the potential to offer an economically viable solution for the recovery of hydrogen from such mixtures. BaZr1−x−yCexYyO3−δ is increasingly regarded as an optimal perovskite hydrogen permeable membrane. Nevertheless, the main drawback to its use in a larger scale is the extremely low hydrogen permeability and stability. An original perovskite material is proposed in this study, BaZr0.7Ce0.2Y0.1O3−δ‐Fx. A thermodynamic‐controlled sintering strategy (TCS) has been employed to inhibit the evaporation of metals from ceramic solids. The TCS directly caused the hydrogen permeation flux to reach 1.07 ml·min−1 cm−2, representing a fourfold improvement. Furthermore, F‐doping demonstrated enhanced performance at low and medium temperatures. The aforementioned successful strategy provides an effective path for the tailoring of perovskite materials and promotes its application for the industrial‐scale separation of hydrogen.