A method of making property modulated composite materials includes depositing a first layer of material having a first microstructure/nanostructure on a substrate followed by depositing a second layer of material having a second microstructure/nanostructure that differs from the first layer. Multiple first and second layers can be deposited to form a composite material that includes a plurality of adjacent first and second layers. By controlling the microstructure/nanostructure of the layers, the material properties of the composite material formed by this method can be tailored for a specific use. The microstructures/nanostructures of the composite materials may be defined by one or more of grain size, grain boundary geometry, crystal orientation, and a defect density.