AbstractMagnetic skyrmions are localized nanometer-sized spin configurations with particle-like properties, which are envisioned to be used as bits in next-generation information technology. An essential step toward future skyrmion-based applications is to engineer key magnetic parameters for developing and stabilizing individual magnetic skyrmions. Here we demonstrate the tuning of the non-collinear magnetic state of an Fe double layer on an Ir(111) substrate by loading the sample with atomic hydrogen. By using spin-polarized scanning tunneling microscopy, we discover that the hydrogenated system supports the formation of skyrmions in external magnetic fields, while the pristine Fe double layer does not. Based on ab initio calculations, we attribute this effect to the tuning of the Heisenberg exchange and the Dzyaloshinsky–Moriya interactions due to hydrogenation. In addition to interface engineering, hydrogenation of thin magnetic films offers a unique pathway to design and optimize the skyrmionic states in low-dimensional magnetic materials.