The design and development of high-efficiency and non-noble metal hydrogen evolution reaction (HER) electrocatalysts with optimized nanostructures for human clean and sustainable energy systems has attracted significant research interest over the past years. Herein, self-supported semimetallic tungsten diphosphide nanowire arrays on carbon cloth (WP2 NWs/CC) were topotactically fabricated by in situ phosphidation of a WO3 NWs/CC precursor. Such a binder-free flexible HER cathode with integrated three-dimensional nanostructures can not only provide a large surface area to expose abundant active sites, but also facilitate electrolyte penetration for electrons and electrolyte ions. The WP2 NWs/CC electrode exhibits superior catalytic performance, and it needs overpotentials of 109 and 160 mV with a small Tafel slope of 56 mV dec-1 to achieve current densities of 10 and 50 mA cm-2, respectively. High stability in acidic media is also observed for the catalyst for a duration of 20 hours at least. In addition, density functional theory (DFT) calculations indicate a low kinetic energy barrier for H atom adsorption on the WP2 surface which guarantees the excellent catalytic activity of the catalyst, and the influences of phosphidation temperature on the HER activity are also studied. The excellent electrocatalytic activity makes the present 3D structured WP2 NWs/CC a promising catalyst for large scale highly pure hydrogen evolution by electrochemical water splitting.