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The design of multifunctional alloys with multiple chemical components requires controllable synthesis approaches. Physical vapor deposition techniques, which result in thin films (<1 μm), have previously been demonstrated for micromechanical devices and metallic combinatorial libraries. However, this approach deviates from bulk-like properties due to the residual stress derived in thin films and is limited by total film thickness. Here, we report a route to obtain ternary Ni-Mn-Sn alloy thick films with controllable compositions and thicknesses by annealing electrochemically deposited multi-layer monatomic (Ni, Mn, Sn) films, deposited sequentially from separate aqueous deposition baths. We demonstrate (1) controllable compositions, with high degree of uniformity, (2) smooth films, and (3) high reproducibility between film transformation behavior. Our results demonstrate a positive correlation between alloy film thicknesses and grain sizes, as well as consistent bulk-like transformation behavior.