Aerosol jet printing (AJP) is an advanced manufacturing technique for directly writing nanoparticle inks onto target substrates. It is an emerging reliable, efficient, and environmentally friendly fabrication route for thin film electronics and advanced semiconductor packaging. This fabrication technique is highly regarded for its rapid prototyping, the flexibility of design, and fine feature resolution. Nickel is an attractive high-temperature packaging material due to its electrical conductivity, magnetism, and corrosion resistance. In this work, we synthesized nickel nanoparticles and formulated an AJP ink, which was printed on various material surfaces. Thermal sintering experiments were performed on the samples to explore the redox behavior and to optimize the electrical performance of the devices. The nickel devices were heated to failure under an argon atmosphere, which was marked by a loss of reflectance and electrical properties due to the dewetting of the films. Additionally, a reduction mechanism was observed from these studies, which resembled that of nucleation and coalescence. Finally, multilayer graphene was grown on a custom-printed nickel thin film using chemical vapor deposition (CVD), establishing a fully additive manufacturing route to patterned graphene.