Herein, using the systematic experimental characterization and density functional theory calculations, the effects of Ni elemental substitution on the crystal structure, cation distribution, magnetic properties, and heat generation ability of Mg1–xNixFe2O4 (x = 0, 0.2, 0.4, 0.6, 0.8, and 1) have been reported. We demonstrate that the presence of Ni can lead the lattice shrinkage, phase transition from partially to fully inverse spinel structure, and multi-domain structures in the samples. Moreover, Ni substitutional atoms make magnetically harder ferrite, associated with increasing magnetic inhomogeneity. Remarkably, anomalous enhancements of magnetic anisotropic and coercivity have been observed in Mg0.4Ni0.6Fe2O4. Heat generation ability (SAR) increases from 242 W g−1 for x = 0–391 W g−1 for x = 0.6 at an AC magnetic field of 370 kHz frequency. Thus, the magnetic hyperthermia of Mg0.4Ni0.6Fe2O4 sample on HeLa shows promising results that the viability of cells decreases to 25 % after 5 sessions. The present experimental and theoretical systematic studies provide novel avenue and paradigm for the development of ferrite nanoparticles with high heat generation ability and magnetic properties for biomedical applications.
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