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The single-phase multiferroic Bi 5 Fe 1−x Ni x Ti 3 O 15 (BFNT-x, x = 0, 0.1, 0.2, 0.3, 0.4, and 0.5) ceramics were synthesized by a sol-gel auto-combustion method, and their microstructures, ferroelectric, magnetic, and dielectric properties were investigated in detail. All samples belong to layer-perovskited Aurivillius phase containing four perovskite units sandwiched between two Bi-O layers. Ni substitution can not only improve ferroelectricity but also enhance the magnetic properties. The BFNT-0.2 sample shows the largest remnant polarization (2P r ∼ 11.6 µC/cm 2 ) and the highest remnant magnetization (2M r ∼ 0.244 emu/g). The enhancement of the magnetic properties may mainly originate from the spin canting of Fe/Ni-O octahedra via Dzyaloshinskii-Moriya (DM) interaction. In order to explore the influence of valance state of magnetic ions on the properties, the x-ray photoelectron spectroscopy was carried out. Furthermore, structural, ferroelectric, and magnetic transitions were also investigated.