Microfluidics, with its remarkable capacity to manipulate fluids and droplets at the microscale, has emerged as a powerful platform in numerous fields. In contrast to conventional closed microchannel microfluidic systems, free‐boundary microfluidic manufacturing (FBMM) processes continuous precursor fluids into jets or droplets in a relatively spacious environment. FBMM is highly regarded for its superior flexibility, stability, economy, usability, and versatility in the manufacturing of advanced materials and architectures. In this review, a comprehensive overview of recent advancements in FBMM is provided, encompassing technical principles, advanced material manufacturing, and their applications. FBMM is categorized based on the foundational mechanisms, primarily comprising hydrodynamics, interface effects, acoustics, and electrohydrodynamic. The processes and mechanisms of fluid manipulation are thoroughly discussed. Additionally, the manufacturing of advanced materials in various dimensions ranging from zero‐dimensional to three‐dimensional, as well as their diverse applications in material science, biomedical engineering, and engineering are presented. Finally, current progress is summarized and future challenges are prospected. Overall, this review highlights the significant potential of FBMM as a powerful tool for advanced materials manufacturing and its wide‐ranging applications.This article is protected by copyright. All rights reserved