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The magnetoelectric (ME) effect, which involves the interaction of magnetic and electric fields within a material, has a significant potential for various applications. Our study addresses the limitations of conventional magnetostriction-based ME materials by demonstrating an alternative approach that achieves substantial ME effects in core-shell-type nanocomposites at room temperature. By synthesizing ferrimagnetic Fe 3 O 4 nanoparticles onto piezoelectric poly(vinylidene fluoride) (PVDF) particles, we identified a distinct ME mechanism. In magnetorheological (MR) fluids, the magnetic-field-induced aggregation of Fe 3 O 4 nanoparticles, combined with the piezoelectricity of PVDF, leads to a pronounced ME effect, significantly enhancing the performance and stability of MR fluids. This research highlights a crucial observation of distinct ME effects, which could suggest potential pathways for advancements in practical applications including microfluidics, vibration dampers, tactile technologies, and biomedical and bioengineering fields.