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The data presented in this article are related to the formation of a novel layered perovskite oxide material, PrSrMn₂O_5+δ, through a solid-state synthesis route. Here, we present the high-resolution neutron powder diffraction and the X-ray powder diffraction data at room temperature. The new perovskite material crystallizes in the orthorhombic symmetry. Interpretation of this data can be found in a research article titled “Insight of novel layered perovskite PrSrMn²O^5+δ: A neutron powder diffraction study” (Shammya et al., 2019) [1].