© 2020 Realizing improved strength in composite metallic materials remains a challenge using conventional welding and joining systems due to the generation and development of brittle intermetallic compounds caused by complex thermal profiles during solidification. Here, wire arc additive manufacturing (WAAM) process was used to fabricate a steel-nickel structural component, whose average tensile strength of 634 MPa significantly exceeded that of feedstock materials (steel, 537 MPa and nickel, 455 MPa), which has not been reported previously. The as-fabricated sample exhibited hierarchically structural heterogeneity due to the interweaving deposition strategy. The improved mechanical response during tensile testing was due to the inter-locking microstructure forming a strong bond at the interface and solid solutions strengthening from the intermixing of the Fe and Ni increased the interface strength, beyond the sum of parts. The research offers a new route for producing high-quality steel-nickel dissimilar structures and widens the design opportunities of monolithic components, with site-specific properties, for specific structural or functional applications.