For the Internet of Underwater Things (IoUT), a large-capacity communication mechanism with high mobility is crucial to achieving information interaction at both short and medium ranges. In addition, to alleviate the energy anxiety of IoUT devices, a mobility enhanced simultaneous underwater optical wireless communication (UOWC) and energy harvesting system is proposed and experimentally demonstrated in this article. Compared with traditional UOWC systems, we first employ light-emitting diode arrays and solar panels as system transceivers, which can not only realize high-speed data transmission without complex alignment operations but also achieves efficient energy harvesting. An experimental demonstration system with a channel length of 0.5 m is established and the energy harvesting and communication performance of the proposed system are analyzed under four typical water types. For the harvesting part, the optimal load resistance is measured for better charging efficiency. The maximum output power measured in pure water is 1.6 times more than that in turbid seawater. For the communication part, with a hardware pre-equalization circuit, the −3-dB bandwidth of the system is increased from 2.3 to 14 MHz. The on–off-keying (OOK) modulation signals with a maximum data rate of 19 Mb/s are successfully transmitted through different water types. Furthermore, the proposed system can achieve reliable communication at data rates greater than 16 Mb/s with a wide 90° field of view, which greatly improves the system response range. The proposed simultaneous UOWC and energy harvesting system shows great potential for the construction of high-dynamic and energy-efficient IoUT networks.