The escalating demand for high-performance soft magnetic materials with exceptional strength is driven by their critical role in energy conversion applications such as electric motors, transformers, and generators. Conventional materials and designs often face limitations and lack the desired properties required for the development of next-generation electric vehicles and wind turbines. Additive manufacturing (AM) technology enables the rapid synthesis of material libraries and the subsequent assessment of multiple properties. We employed laser additive manufacturing techniques, direct energy deposition (DED) and/or laser powder bed fusion (LPBF), to produce Fe-Co-Ni, Fe-Co-Ni-xAl, and Fe-xSi alloys. Laser process parameters optimization and the microstructures, magnetic, electrical, and mechanical properties of these materials were investigated. These newly developed materials exhibited exceptional and tunable properties. Such tunable functionality offers a unique opportunity to select materials according to specific applications, particularly for high-speed electric machines. Moreover, the impact of laser energy and annealing on the microstructure, grain orientation, and anisotropy of magnetic properties of these materials was studied. A significant change in these properties was observed when they were processed by DED or LPBF. For instance, DED-processed Fe-3.8Si showed substantially coarser columnar grains and exhibited 50% lower coercivity values compared to their LPBF counterparts. AM can provide new opportunities for developing novel magnetic components with improved performance, contributing to the advancement of various industries relevant to electrification and energy conversion.