One of the challenges in making layered metal composites reinforced at interfaces has been controlling the dispersion and microstructure of the reinforcement particles. The reinforcement elements are typically applied at the interface by manual spreading using brush or by immersing the substrate in a suspension. In this study, an ultrasonic spraying technique has been used to deposit silicon carbide (SiC) nanoparticles on aluminum 6061 (Al6061) substrate foils to fabricate a laminate metal composite to control the deposited structure. The suspension parameters and the spraying parameters were investigated, and their influence on the deposited microstructure was analyzed. The laminate composite was consolidated using hot compaction, and a three-point bend test was performed to evaluate the mechanical properties. The yield and ultimate flexural strengths of the laminate composite reinforced with SiC nanoparticles increased by 32% and 15%, respectively, compared with those of the unreinforced sample prepared at the same condition.