Phosphor-free InGaN/AlGaN core-shell nanowire light-emitting diodes (LEDs) grown by molecular beam epitaxy have been developed and their application in visible light communication (VLC) has been investigated. The electroluminescence spectra of these nanowire LEDs show a very broad spectral linewidth and fully covers the entire visible spectrum. High-brightness phosphor-free LEDs with highly stable white-light emission and high color-rendering index (CRI) of >98 were obtained by controlling the Indium composition in the device active region. Moreover, the phosphor-free nanowire white-LEDs exhibit relatively high 3-dB frequency bandwidth of ∼ 1.4 MHz which is higher compared to that of phosphor-based white LEDs at the same measurement condition. Such high-performance phosphorfree nanowire LEDs are being further improved and are ideally suited for future smart lighting applications and communications.