Low-field intergrain magnetoresistance (IMR) in the polycrystalline materials of double perovskite SrFe0.5Mo0.5O3 is found to be highly tunable by doping either Ca or Ba into the Sr site. The dopant exerts a chemical pressure, changing the Curie temperature and the magnetic softness. The room-temperature IMR at optimal doping (Sr0.2Ba0.8Fe0.5Mo0.5O3) is approximately 3.5% in 100 Oe, and increases further in high fields. The unprecedented magnitude of the IMR in this highly spin polarized system provides future grounds for employing magnetic materials for innovative magnetic technology.

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