AbstractThe established approach to materials design for additive manufacturing (AM) consists of attempting to reproduce the uniform structures and properties of conventionally processed materials. While this certainly helped facilitate material certification and the rapid introduction of AM technologies in several industries, the opportunity to exploit unique features of specific AM processes to generate spatially varying microstructures–and hence novel materials, remains largely untapped. This work presents a method for manufacturing materials through laser powder bed fusion (LPBF), in which control over the spatial variation in phase composition and mechanical properties is achieved. This technique is demonstrated using 17‐4 precipitation‐hardened stainless steel (17‐4PH), by controlling spatial modulation of energy densities during printing. This results in local control of ferrite/martensite volume fractions, allowing the fabrication of metal/metal architected composites with hard/brittle regions interspersed with soft/tough regions. Local variations of ~20% in tensile strength and ~150% in elongation are achieved, with a spatial resolution of ~100 microns. The approach is general and robust, fully compatible with commercially available LPBF equipment, and applicable to virtually any multi‐phase alloy system. This work shifts the paradigm from attempting to print components with uniform properties to manufacturing alloys with controlled spatial property gradients.