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The important benefits of ultrafine-grained (UFG) alloys for various applications stem from their enhanced superplastic properties. However, decreasing the temperature of superplasticity and providing superplastic forming at lower temperatures and higher strain rates is still a priority. Here, we disclose, for the first time, the mechanism by which grain boundary sliding and rotation are enhanced, when UFG materials have grain boundary segregation of specific alloying elements. Such an approach enables achieving superplasticity in commercial Al alloys at ultralow homologous temperatures below 0.5 (i.e. below 200°C), which is important for developing new efficient technologies for manufacturing complex-shaped metallic parts with enhanced service properties.