The light-emitting diode nonlinearity in visible light communication (VLC) systems is considered to be a major problem that deteriorates system performance. In this paper, we experimentally demonstrate a high-speed WDM CAP64 VLC system employing a Volterra series-based nonlinear equalizer to mitigate the nonlinear effect. A modified cascaded multimodulus algorithm (M-CMMA) is utilized to calculate the error function and update the weights of the nonlinear equalizer without using training symbols. An aggregate data rate of 4.5 Gb/s is successfully achieved over 2-m indoor freespace transmission with a bit error rate (BER) below the 7% forward error correction limit of 3:8 Â 10 À3 . With the Volterra nonlinear equalizer, the Q factor of the VLC system is 1. 6 dB better than that without using the nonlinear equalizer, and the transmission distance is also increased by about 110 cm at the BER of 3:8 Â 10 À3 . To the best of our knowledge, this is the first time that the Volterra nonlinear equalizer is utilized for highspeed carrierless amplitude and phase (CAP) modulation-based VLC systems.