Nanoparticle-included polymeric composite coatings with preferential nanoparticle alignment and oriented structures show improved functional and structural properties than randomly oriented structures, suitable for broad applications in microelectronics, automobile, defense, and space missions. Traditionally used techniques, such as drop-casting, chemically modified surfaces, and external fields, have been used for selfassembly but with several disadvantages, such as material limitations. Thus, there is a need to develop a new approach for generating hierarchical nanoparticle structures. Our unique processing is based on advanced additive manufacturing with a colloidal suspension-based deposition approach for layer-bylayer deposition of anisotropic nanoparticles. Leveraging the colloidal deposition technique, these anisotropic nanoparticles were deposited onto the 3D printed substrates with designed patterning. The presence of micropatterns generates selective nanoparticle distribution and assembly along with hydrodynamic forces to initiate the region-specific microscale patterning and nanoscale alignment of 1D and 2D nanoparticles. The polymer and nanoparticle composite film showed different deposition morphologies (e.g., straight or wavy films). In addition, the influence of nanoparticle deposition morphology on functional properties was investigated. This novel technique shows the potential to scale up microelectronics production by 3D printing electronic structures, including interdigitated devices, supercapacitors, fuel cells, and circuits.