We demonstrate very high frequency (VHF) nanomechanical resonators based upon single-crystal silicon nanowires (SiNWs), which are prepared by the bottom-up chemical synthesis. Metallized SiNW resonators operating near 200 MHz are realized with quality factor Q ≈ 2000−2500. Pristine SiNWs, with fundamental resonances as high as 215 MHz, are measured using a VHF readout technique that is optimized for these high resistance devices. The pristine resonators provide the highest Q's, as high as Q ≈ 13 100 for an 80 MHz device. SiNWs excel at mass sensing; characterization of their mass responsivity and frequency stability demonstrates sensitivities approaching 10 zeptograms. These SiNW resonators offer significant potential for applications in resonant sensing, quantum electromechanical systems, and high frequency signal processing.Nanoelectromechanical systems (NEMS), particularly nanomechanical resonators vibrating at high frequencies, 1 are being actively explored for applications including resonant sensors for ultrahigh-resolution mass sensing, 2 force detection, 3 quantum electromechanics, 4 electromechanical signal generation and processing, 5 and high-speed logic and computation. 6 These NEMS resonators are usually made by topdown lithographic techniques and surface nanomachining, which together enable realization of nanomechanical devices with considerable complexity and functionality. By contrast, chemical-synthesis-based bottom-up approaches now provide nanowires with high crystalline quality, perfectly terminated surfaces, and sizes down to the molecular scale. These represent a new class of building blocks for NEMS resonators that offer unique attributes. Si nanowires (SiNWs) are, perhaps, among the most intriguing given silicon's preeminent role in micro-and nanoelectronics and as a structural material for micro-and nanoelectromechanical systems. Development of SiNW-NEMS, however, has been impeded by difficulties in suspending SiNWs to give them mechanical freedom and in subsequent device integration. Recently, a hybrid process has been developed to fabricate SiNWs suspended over microtrenches by employing vapor-liquidsolid (VLS) epitaxial growth.8 This device geometry facilitates the direct probing of mechanical properties of SiNWs via static deflection. 9,10 In this Letter, we describe the first demonstration of resonant mechanical devices operating at very high frequencies (VHF) that are based on such suspended SiNWs. We demonstrate robust SiNW resonators vibrating at frequencies greater than 200 MHz. Furthermore, comprehensive measurements of the resonance characteristics, quality factors, and resonator frequency stability show that these bottom-up SiNWs provide excellent performance. These devices expand and advance prospects for NEMS resonator technologies and enable new possibilities for applications. Parts a and b of Figure 1 show the typical suspended SiNWs in microtrenches. The detailed synthetic procedure via VLS epitaxial growth has been described in ref 8. Briefly, the SiNW begins cry...