Inspired by the catalytic activity along the edge sites of layeredstructured MoS 2 for the hydrogen evolution reaction (HER), maximizing the specific active edge sites per unit geometric area via material architectural design is the most common strategy for enhancing HER performance. Here, we report a convenient growth approach using atomic layer deposition (ALD) to obtain novel nanostructures of MoS 2 nanotube arrays with a high number of exposed active edge sites. MoS 2 NTs were spontaneously immobilized in an ordered arrangement of anodic aluminum oxide (AAO) template with a well-defined size and shape. Ordered MoS 2 NTs array were fabricated with highly conductive, large electrochemical active area as an efficient HER catalyst. Strikingly, by engineering the contact metal serving as the current collector, the contact properties were revealed to be important factors for the electrocatalytic performance of the metal-assisted MoS 2 electrodes. Our material system shows a significantly low overpotential of 260 mV at 10 mA/cm 2 and a Tafel slope of 55 mV/dec, while it remains stable during longterm operation in strong acidic media.