Despite the rapidly growing amount of knowledge on the structure and function of cells, they remain a distant bottom-up synthetic target due to their overwhelming complexity. A path to this goal is the development of protocellular systems that approximate one or more aspects of a natural cell. Polymer vesicles, or polymersomes, are an attractive scaffold for protocellular constructs, due to our ability to engineer the polymer membrane and generate a wide range of properties. This article summarizes the current state of polymersome science with respect to the properties and functions that lend these polymer-based systems to applications in synthetic cell research. (C) 2017 Wiley Periodicals, Inc.