Significant leaps in the understanding of quantum systems have been driven by the exploration of geometry, topology, dimensionality, and interactions with ultracold atomic ensembles. A system where atoms evolve while confined on an ellipsoidal surface represents a heretofore unexplored geometry and topology. Realizing such an ultracold bubble system (potentially Bose-Einstein condensed) has areas of interest including quantized-vortex flow respecting topological constraints imposed by closed surfaces, new collective modes, and self-interference via free bubble expansion. Large ultracold bubbles, created by inflating smaller condensates, directly tie into Hubble-analog expansion physics. Here, we report observations from the NASA Cold Atom Lab facility aboard the International Space Station of bubbles of ultracold atoms created using a radiofrequency-dressing protocol. We observe a variety of bubble configurations of differing sizes and initial temperature, and explore bubble thermodynamics, demonstrating significant cooling associated with inflation. Additionally, we achieve partial coverings of bubble traps greater than 1 mm in size with ultracold films of inferred few-$mu$m thickness, and we observe the dynamics of shell structures projected into free-evolving harmonic confinement. The observations are part of the first generation of scientific measurements made with ultracold atoms in space, exploiting the benefits of perpetual free-fall to explore gravity-free evolution of quantum systems that are prohibitively difficult to create on Earth. This work points the way to experiments focused on the nature of the Bose-Einstein condensed bubble, the character of its excitations, and the role of topology in its evolution; it also ushers in an era of orbital microgravity quantum-gas physics.