High spectral efficiency is a key element that drives research for future wireless communication systems in order to meet the increasing demand for ubiquitous connectivity despite a limited radio frequency spectrum. Visible light communications (VLC) that allow exploiting the existing infrastructure for both lighting and communications could be an effective and economic solution. Thanks to the revolution in the field of solid-state lighting and the accelerated development of light-emitting diodes (LED), VLC becomes one of the most promising new technologies for the next generation of wireless communication systems. However, the limited bandwidth of the LEDs remains a major challenge that is limiting VLC from achieving very high data rates. In this paper, we propose to adapt the discrete multi-tone (DMT) modulation scheme of indoor VLC communications for data rate enhancement. With the help of bit and power-loading algorithms, a transmission bandwidth much larger than the 3-dB bandwidth of the LED could be exploited. We firstly present the typical lighting requirements for indoor applications and investigate the maximal bit-rate of DMT-based VLC. Then, with a regular luminance level for normal office work, an overall optimization of DMT configuration scheme in terms of modulated bandwidth, subcarrier number, cyclic prefix length, and clipping level is proposed. Theoretical analysis and verifications by experiments are simultaneously carried out. Based on the proposed configuration, we demonstrate a 100-Mbps VLC wireless transmission employing low-cost components under realistic lighting constraints.