Topological materials are derived from the interplay between symmetry and topology. Advances in topological band theories have led to the prediction that the antiperovskite oxide Sr3SnO is a topological crystalline insulator, a new electronic phase of matter where the conductivity in its (001) crystallographic planes is protected by crystallographic point group symmetries. Realization of this material, however, is challenging. Guided by thermodynamic calculations, a deposition approach is designed and implemented to achieve the adsorption-controlled growth of epitaxial Sr3SnO single-crystal films by molecular-beam epitaxy (MBE). In situ transport and angle-resolved photoemission spectroscopy measurements reveal the metallic and electronic structure of the as-grown samples. Compared with conventional MBE, the used synthesis route results in superior sample quality and is readily adapted to other topological systems with antiperovskite structures. The successful realization of thin films of Sr3SnO opens opportunities to manipulate topological states by tuning symmetries via strain engineering and heterostructuring. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim