Molybdenum disulfide (MoS2) as a representative transition-metal dichalcogenide (TMD) has been extensively used as a noble-metal-free cocatalyst for photocatalytic hydrogen (H-2) production, but suffers from poor photocatalytic activity due to the catalytic inactivity of its basal plane. Herein, by bounding another metal-free cocatalyst, C-60, with MoS2, we report the first MoS2-C-60 hybrid featuring a van der Waals heterostructure prepared via a facile and eco-friendly solid-state mechanochemical route. C-60 bounding onto the edge of MoS2 nanosheets leads to the decreases of both the number of layers and the size of MoS2 nanosheets, as well as a negative shift of the conduction band minimum along with a positive shift of valance band maximum relative to the bulk MoS2 and MoS2 ball-milled without C-60 (MoS2-BM). Under the optimized weight ratio of MoS2:C-60 (1:1) in the raw mixture subject to ball-milling, MoS2-C-60 hybrid containing 2.8 wt% C-60 shows an exceptional visible light photocatalytic H-2 production rate of 6.89 mmol h(-1) g(-1) in the presence of a photosensitizer Eosin Y (EY), which is significantly enhanced relative to the bulk MoS2 and pristine C-60, both of which show almost no photocatalytic H-2 activity. Thus, the synergistic enhancement of photocatalytic activities of both MoS2 and C-60 is revealed. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.