Manganese ferrite (MnFe2O4) nanoparticles initially fabricated using a solvothermal process were coated with conducting polyaniline (PANI) to produce core/shell-structured MnFe2O4/PANI nanoparticles. An electro/magnetorheological (E/MR) fluid was prepared by suspending MnFe2O4/PANI particles in silicone oil, and the rheological properties under either electric or magnetic fields were investigated. Scanning electron microscope and transmission electron microscope provided the particle morphology and size information. X-ray diffraction and Fourier transform infrared spectroscopy were used to analyze the crystal structure and chemical composition of the particles. Chain formation in E/MR fluids under electric or magnetic fields was observed by optical microscopy, and the rheological properties were evaluated using a rheometer. Steady shear and dynamic oscillatory tests were conducted to confirm the effective E/MR characteristics while varying the electric/magnetic field strength. The dielectric properties of the particles measured using an LCR meter were analyzed based on the Cole-Cole model. The E/MR fluids composed of MnFe2O4/PANI showed a reversible and fast electro/magnetic response.