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MoS 2 nanomaterials show excellent high theoretical performance in energy storage and hydrogen evolution reaction (HER), whereas they typically suffer from agglomeration and poor electrical conductivity. In this study, unique few-layer molybdenum disulfide nanosheet/carbon nanotube (MoS 2 /CNT) films are fabricated via an electrochemical exfoliation method. On the one hand, owing to the coupling effects of well-dispersed few-layer MoS 2 nanosheets and excellent conductive CNTs, these stateof-the-art films not only afford a short ion-diffusion distance and a fast electron-transport path but also provide abundant active sites and maximized reaction interfaces as well. On the other hand, these free-standing films are capable of being directly used as electrodes without requiring additives, endowing the clean interfaces with reduced charge-transfer resistance. As a result, the few-layer MoS 2 /CNT films demonstrate a much lower capacity decay rate (0.01%) over 8000 cycles as an anode material of Li-ion batteries and superior hydrogen generation performance with an optimal Gibbs free energy for hydrogen adsorption (ΔG H* ) as a catalyst of HER, in contrast to the various MoS 2 -based nanomaterials.