The next generation of space structures demands unprecedented multifunctionality, incorporating capabilities to morph, adapt, sense, communicate, generate and manage energy, and process information. Realizing ultra-large space infrastructures, such as space solar farms, orbital data centers, and human habitats, requires breakthrough advances in in-space structural assembly and manufacturing (ISAM). This presentation will highlight several projects aimed at these ambitious, long-term goals. I will first present our work on multifunctional flexible space structures integrated with soft electronics, followed by an in-depth discussion of the mechanics of bistable ultrathin composite booms. The presentation will also include brief introduction to our group’s state-of-the-art Low-Earth Orbit environment simulation facility. The talk will conclude with our recent research on structural interfaces and joints for in-space assembly, as well as extravehicular additive manufacturing of continuous carbon fiber-reinforced thermoplastics.