This paper demonstrates an easily prepared novel material and approach to producing aligned nickel (Ni) nanowires having unique and customizable structures on a variety of substrates for electronic and magnetic applications. This is a new approach to producing printed metallic Ni structures from precursor materials, and it provides a novel technique for nanowire formation during reduction. This homogeneous solution can be printed in ambient conditions, and it forms aligned elemental Ni nanowires over large areas upon heating in the presence of a magnetic field. The use of templates or subsequent purification are not required. This technique is very flexible, and allows the preparation of unique patterns of nanowires which provides opportunities to produce structures with enhanced anisotropic electrical and magnetic properties. An example of this is the unique fabrication of aligned nanowire grids by overlaying layers of nanowires oriented at different angles with respect to each other. The resistivity of printed and cured films was found to be as low as 560 µ?·cm. The saturation magnetization was measured to be 30 emu·g−1, which is comparable to bulk Ni. Magnetic anisotropy was induced with an axis along the direction of the applied magnetic field, giving soft magnetic properties.