One-dimensional transition metal dichalcogenides exhibiting an enhanced bulk photovoltaic effect have the potential to exceed the Shockley–Queisser limit efficiency in solar energy harvest within p - n junction architectures. However, the collective output of these prototype devices remains a challenge. We report on the synthesis of single-crystalline WS 2 ribbon arrays with defined chirality and coherent polarity through an atomic manufacturing strategy. The chirality of WS 2 ribbon was defined by substrate couplings into tunable armchair, zigzag, and chiral species, and the polarity direction was determined by the ribbon-precursor interfacial energy along a coherent direction. A single armchair ribbon showed strong bulk photovoltaic effect and the further integration of ~1000 aligned ribbons with coherent polarity enabled upscaling of the photocurrent.