In general, visible light communication (VLC) systems, which utilise white light-emitting diodes (LEDs), only offer a bandwidth limited to the lower MHz region. Therefore, providing VLC-based high data rate communications systems becomes a challenging task. To address this challenge, we propose a solution based on multiplexing in both the frequency and space domains. We experimentally demonstrate a 4 × 4 imaging multiple-input multiple-output (MIMO) VLC system (i.e., space multiplexing) utilising multi-band carrier-less amplitude and phase (m-CAP) modulation (i.e., frequency multiplexing). Independently, both MIMO and m-CAP have shown the remarkable ability to improve transmission speeds in VLC systems, and hence, here we combine them to further improve the net data rate. We investigate link performance by varying the number of subcarriers m, link distance L, and signal bandwidth Bsig. From all the values tested, we show a data rate of ~249 Mb/s can be maximally achieved for for m = 20, Bsig = 20 MHz, and L = 1 m, at a bit error rate of 3.2×10-3 using LEDs with ~4 MHz bandwidth. Index Terms-Modulation bandwidth, multi-band carrier-less amplitude and phase modulation, multiple-input multiple-output, visible light communications.