To increase the traffic rate in phosphor-LED visible light communication (VLC), a multi-band orthogonal frequency division multiplexed (OFDM) modulation is first proposed and demonstrated. In the measurement, we do not utilize optical blue filter to increase modulation bandwidth of phosphor-LED in the VLC system. In this proposed scheme, different bands of OFDM signals are applied to different LED chips in a LED lamp, this can avoid the power fading and nonlinearity issue by applying the same OFDM signal to all the LED chips in a LED lamp. Here, the maximum increase percentages of traffic rates are 41.1%, 17.8% and 17.8% under received illuminations of 200, 500 and 1000 Lux, respectively, when the proposed three-band OFDM modulation is used in the VLC system. In addition, the analysis and verification by experiments are also performed.