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Accelerated development of soft magnetic materials is vital for addressing the challenges associated with improving the performance of electrical machines, transformer cores, electric vehicles etc. A combinatorial assessment of the structural, magnetic and mechanical properties of Co_100-xFe_x (x = 30 to 70) and Ni_100-xFe_x (x = 30 to 70) alloys has been carried out on samples fabricated via laser additive manufacturing (AM). Co_100-xFe_x showed a bcc structure in the composition range studied while Ni_100-xFe_x exhibited either single phase fcc or a mixture of fcc and bcc phases, depending on the composition. The saturation magnetization (M_s) for both Co_100-xFe_x and Ni_100-xFe_x compositionally graded alloys increases monotonically with increasing Fe content while the coercivity (H_c) variation is not monotonic. The M_s value of 199.3 emu/g for Co₇₀Fe₃₀ increases to 248 emu/g for Co₃₀Fe₇₀ alloys. Ni₇₀Fe₃₀ …