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This article reports a new approach toward fabrication and directed assembly of nanoparticulate reactive system (Nanofoils) on patterned substrates. Different from current state‐of‐the‐art, gas phase electrodeposition uses nanoparticles instead of atoms to form densely packed multilayered thin films at room temperature‐pressure. On ignition, the multilayer system undergoes an exothermic self‐propagating reaction. The numerous contact points between two metallic nanoparticulate layers aid in high heat release. Sub‐10‐nm Platinum (Pt) and Aluminum (Al) particles are synthesized through cathode erosion of metal electrodes in a flow of pure nitrogen gas (spark ablation). Pt/Al bilayer stacks with total thickness of 3–8 µm undergo self‐propagating reaction with a 10.3 mm s−1 wavefront velocity on local ignition. The reaction wavefront is captured using high speed videography. Calorimetry studies reveal two exothermic peaks suggesting Pt/Al alloy formation. The peak at 135 °C has a higher calorific value of 150 mW g−1 while the peak at 400 °C has a 12 mW g−1 exothermic peak. X‐ray diffraction study shows reaction‐products are cubic Al2Pt with small quantities of orthorhombic Al6Pt and orthorhombic AlPt2. Electron microscopy studies help draw a correlation between film morphology, bimetallic interface, nanoparticle oxidation, and self‐propagating reaction kinetics that is significant in broadening our understanding towards nanoparticulate reactive systems. [ABSTRACT FROM AUTHOR]