• Ni doping at A-site (Sm1−xNixCrO3) significantly enhances low-temperature magnetic properties, with Sm0.80Ni0.20CrO3 showing up to 93.5% increase in field-cooling magnetization at 100 Oe.
• A-site Ni doping outperforms B-site doping at equivalent ratios, yielding higher magnetization, lower dielectric loss, and improved electrical quality factors.
• All Ni-doped ceramics retain orthorhombic Pbnm structure, and Ni ions exist as Ni2+ as confirmed by XPS.
• The study provides a structure-activity relationship for optimizing magnetic and dielectric properties in SmCrO3-based ceramics for potential applications in electronic and spintronic devices.
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