The rapidly growing demand for data storage and processing, driven by artificial intelligence (AI) and other data-intensive applications, is posing a serious challenge for current computing devices based on the von Neumann architecture. For every calculation, data sets need to be shuffled sequentially between the processor, and multiple memory and storage units through bandwidth-limited and energy-inefficient interconnects, typically causing 40% power wastage. Phase-change materials (PCMs) show great promise to break this bottleneck by enabling nonvolatile memory devices that can optimize the complex memory hierarchy, and neuro-inspired computing devices that can unify computing with storage in memory cells. The articles in this issue of MRS Bulletin highlight recent breakthroughs in the fundamental materials science, as well as electronic and photonic implementations of these novel devices based on PCMs.