Union between top-down and bottom-up assembly is inevitable when scaling down physical, chemical, and biological sensors and probes. Current sensor/probe-based technologies are firmly founded on top-down manufacturing, with limitations in cost of production, manufacturing methods, and material constraints. As an alternative to such limitations, contemporary synthesis techniques for one-dimensional nanostructures have been combined with established methods of micro-fabrication for the development of novel tools and techniques for nanotechnology. More specifically, this dissertation is a systematic study of the synthesis and characterization of ZnO nanostructures for piezoelectric applications. Within this study the following goals have been achieved: 1) rational design and control of a diversity of novel ZnO nanostructures, 2) improved understanding of polar-surface-dominated (PSD) phenomena among Wurtzite crystal structures, 3) confirmation of Taskers Rule via the synthesis, characterization, and modeling of polar-surface-dominated nanostructures, 4) measurement of the surface-charge density for real polar surfaces of ZnO, 5) confirmation of the electrostatic polar-charge model used to describe polar-surface-dominated phenomena, 6) dispersion of ZnO nanobelts onto the selective layers of surface acoustic wave (SAW) devices for gas sensing applications, 7) manipulation of ZnO nanostructures using an atomic force microscope (AFM) for the development of piezoelectric devices, 8) fabrication of bulk acoustic resonator (BAR) and film bulk acoustic resonator (FBAR) devices based on the integrity of individual ZnO belts, 9) electrical characterization of a ZnO belt BAR device, 10) prediction and confirmation of the electrical response from a BAR device using a one-dimensional Krimholt-Leedom-Matthaei (KLM) model, and 11) development of a finite element model (FEM) to accurately predict the electrical response from ZnO belt BAR and FBAR devices in 3D.