Inspired by photosynthesis in nature, artificial photosynthesis (AP) systems have been widely investigated in the context of energy and environmental research. Here we report a noble-metal-free AP system for visible-light-driven H-2 generation from aqueous solutions consisting of fluorescein (FL) as photosensitizer, single-layer ultrasmall MoS2 nanoplates embedded in carbon nanofibers (CNF) as electron relay and redox catalyst, and triethanolamine (TEOA) as sacrificial electron donor. This CNF-MoS2/FL system exhibits outstanding H-2 evolution performance, with an H-2 generation rate that exceeds not only both MoS2/FL (by 100%) and CNF/FL (by 1100%), but also the Pt/FL system (by 40%). The excellent photocatalytic activity of this CNF-MoS2/FL system can be ascribed to the synergistic effects of CNF and MoS2 coupling: (1) the simultaneous presence of MoS2 with its delocalized and increased Mo 4d unoccupied states and of CNF with increased graphitic characteristics enables electron transfer from FL* to MoS2 via CNF electron relay; (2) the single-layered ultrasmall MoS2 nanoplates with short effective lengths for electron transfer and high density of reactive S-edges effectively catalyze the H-2 evolution reaction (HER). The presented work successfully fabricated a highly efficient AP system for solar H-2 production from a fully aqueous solution and indicated CNF-MoS2 as a promising candidate to replace Pt for solar fuel conversion. (C) 2017 Elsevier Inc. All rights reserved.