In this chapter, we review our recent works on the phosphor white-light light-emitting diode (LED)-based wireless visible light communication (VLC) and its applications. This chapter is divided into two sections for introduction. In the first section, in order to enhance the transmission rate in phosphor-LED VLC system, we propose and demonstrate a novel multiband orthogonal-frequency-division-multiplexed (OFDM) modulation format for capacity enhancement. Based on the proposed scheme, various bands of OFDM signals are employed to different LED chips of the LED luminary; it can prevent the power fading and nonlinearity effects of transmission signal. Therefore, the maximum enhanced percentage of VLC data rate is 41.1%. In the second section, we also demonstrate a 71.3-148.4 Mbps phosphor-LED wireless VLC system at the free space transmission distance between 1.4 and 2.1 m. Finally, to understand and demonstrate the real-time LED VLC transmission, a commercial OFDM-based digital signal processor (DSP) is used in the LED transmitting side and client side, respectively. Therefore, the proposed real-time half-duplex VLC system can complete around 70 Mbps downstream and upstream traffic throughputs, in a free space transmission distance of 2 m long for practical in-home illumination and smart city applications.