<p>Micro- and nanoparticles (MNP) attract much attention owing to their unique properties, structural tunability, and wide range of practical applications. To deposit these important materials on surfaces for generating functional coatings, a variety of special delivery systems and coating/printing techniques have been explored. Herein, spray coating technique is a promising candidate to advance the field of nanotechnology due to its low-cost, high-deposition rate, manufacturing flexibility, and compatibility with roll-to-roll processing. Despite great advances, direct scalable spray writing of functional materials at high-spatial resolution through fine patterning without a need of vacuum and mask equipment still remains challenging. Addressing these limitations requires the development of efficient spray deposition techniques and novel manufacturing approaches to effectively fabricate functional coatings. To this end, this dissertation employs three different spray coating methods of (1) cold spray; (2) atomization-assisted supersonic spray, and (3) dual velocity regime spray to address the aforementioned limitations. A comprehensive set of coating materials, design principles, and operational settings for each spray system are tailored for rapid, direct, and sustainable deposition of MNP on various substrates. Besides, through the two-phase flow modeling, droplets dispersion and deposition characteristics were investigated under both subsonic and supersonic flow conditions to uncover the process-structure-property relationships of the established spray systems. Moreover, novel spray-based manufacturing approaches are developed to fabricate functional coatings in various applications, including (i) functional polymer metallization, (ii) printed flexible electronics, (iii) advanced thin-film nanocoating, (iv) laser direct writing, and (v) electronic textiles.</p>