jats:titleSignificance</jats:title> jats:pUnderstanding complex materials, in particular those with solid–liquid interfaces, such as water on surfaces or under confinement, is a key challenge for technological and scientific progress. Although established simulation approaches have been able to provide important atomistic insight, ab initio techniques struggle with the required time and length scales, while force field methods can often be limited in terms of their accuracy. Here we show how these limitations can be overcome in a simple and automated machine learning procedure to provide accurate models of interactions at the ab initio level, as illustrated for a variety of complex aqueous systems. These developments open up the prospect of the straightforward exploration of many technologically relevant systems by molecular simulations.</jats:p>