Manipulation at the atomic level: Freestanding SnS2 single-layers with three atom thickness were synthesized through an exfoliation strategy (see picture). The SnS2 single-layers have an increased density of states at the valence band edge. A photoelectrode made from this material shows a visible-light conversion efficiency of 38.7 % that is superior to most existing reports. Detailed facts of importance to specialist readers are published as ”Supporting Information”. Such documents are peer-reviewed, but not copy-edited or typeset. They are made available as submitted by the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Freestanding Tin Disulfide Single‐Layers Realizing Efficient Visible‐Light Water Splitting