The self-propulsion of bodies floating in water is of great interest for developing new robotic and intelligent systems at different scales, and whenever possible, Marangoni propulsion is an attractive candidate for the locomotion of untethered micro-robots. Significant cases have been shown using liquid and solid surfactants that allow an effective propulsion for bodies floating on water to be achieved. Here, we show for the first time a strategy for activating a twofold functionality where the self-propulsion of a floating body is combined with the formation of a polymer thin film at the water surface. In fact, we demonstrate that by using polymer droplets with an appropriate concentration of solvent and delivering such drops at specific locations onto freely floating objects, it is possible to form “on-the-fly” thin polymer films at the free water surface. By exploiting self-propulsion, a polymer thin film can be formed that could cover quite extensive areas with different shapes depending on the motion of the floating object. This intriguing twice-functionality activated though a single phenomenon, i.e., film formation and related locomotion, could be used in perspective to perform complex operations at water surfaces, such as dynamic liquid packaging, cleaning, and moving away floating particles, monolayer films, or macro-sized objects, as discussed in the text.