A water surface not only provides a habitat to many living organisms but also opens up new possibilities to develop state-of-the-art technologies. Here, we show a technology for the layer-by-layer assembly of free-standing nanofilms by controlled rolling. The water surface is exploited as an ideal platform for rolling a nanofilm, allowing adhesion control and frictionless feeding. The nanofilm floating on the water surface is attached to a tube by van der Waals adhesion and is rolled up by the rotation of the tube. This method can assemble diverse film materials including metals, polymers, and two-dimensional materials, with an easy control of the number of layers. Furthermore, heterogeneous and spiral structures of the nanofilm are achieved. Various applications such as a stretchable tubular electrode, an electroactive polymer tube actuator, and a superelastic nanofilm tube are demonstrated. We believe this work can potentially lead to a breakthrough in the nanofilm assembly processes.