An approach to printing a nickel precursor ink on a wide range of substrates for electronics and magnetic applications is disclosed. The nickel ink reduces to elemental nickel following heating. The ink was printed using an ultrasonic aerosol printing technique. By sintering the nickel precursor ink in the presence of a homogeneous magnetic field, the reduced nickel complex formed continuously aligned nickel nanofibers axially aligned with the direction of the magnetic field. The fabrication of aligned interlayered nanofiber films provides opportunities to produce structures with enhanced isotropic electrical and magnetic properties. The resistivity of the film was found to be as low as 0.56 mΩ·cm, and the saturation magnetization was measured to be 30 emu/g, which is comparable to bulk Ni. Magnetic anisotropy was induced with an easy axis along the direction of the applied magnetic field with soft magnetic properties.