Quantum networks promise to revolutionize technology by enabling provably secure communication, ultra-precise sensors for scientific discovery, and new forms of distributed and blind quantum computing. However, current quantum hardware is noisy, error-prone, and inefficient, making the reliable distribution of entanglement -- the key resource powering these applications -- a formidable challenge. This project seeks to overcome these hurdles by developing a novel, comprehensive framework to design and operate quantum networks with maximum efficiency. By creating intelligent control policies that are co-designed with the underlying hardware, this work will enable near-term quantum systems to perform tasks that are currently out of reach. This research serves the national interest by accelerating the development of a secure quantum communication infrastructure, a cornerstone for national defense and economic prosperity. The project’s advancements will also support scientific progress by enabling new instruments, such as quantum-enhanced telescopes, and will foster economic welfare through applications in drug discovery and materials science. The project will produce open-source software tools, benefiting the entire research community. Furthermore, it includes significant educational components, developing new university curricula, supporting undergraduate research, and creating pathways for students to enter the quantum information science workforce. This project's central g