Although the 5G wireless network has made significant advances, it is not enough to accommodate the rapidly rising requirement for broader bandwidth in post-5G and 6G eras. As a result, emerging technologies in higher frequencies including visible light communication (VLC), are becoming a hot topic. In particular, LED-based VLC is foreseen as a key enabler for achieving data rates at the Tb/s level in indoor scenarios using multi-color LED arrays with wavelength division multiplexing (WDM) technology. This paper proposes an optimized multi-color LED array chip for high-speed VLC systems. Its long-wavelength GaN-based LED units are remarkably enhanced by V-pit structure in their efficiency, especially in the “yellow gap” region, and it achieves significant improvement in data rate compared with earlier research. This work investigates the V-pit structure and tries to provide insight by introducing a new equivalent circuit model, which provides an explanation of the simulation and experiment results. In the final test using a laboratory communication system, the data rates of eight channels from short to long wavelength are 3.91 Gb/s, 3.77 Gb/s, 3.67 Gb/s, 4.40 Gb/s, 3.78 Gb/s, 3.18 Gb/s, 4.31 Gb/s, and 4.35 Gb/s (31.38 Gb/s in total), with advanced digital signal processing (DSP) techniques including digital equalization technique and bit-power loading discrete multitone (DMT) modulation format.