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Abstract Rapid and scalable production of high‐performance composites remains a key challenge in achieving sustainable manufacturing. Here, Exo‐press frontal polymerization (EPFP), a novel and transformative method for manufacturing fiber‐reinforced thermoset polymer composites, overcoming energy efficiency, scalability, and curing complex geometries, is introduced. Unlike conventional curing methods that require prolonged processing times and high energy, EPFP utilizes exothermic heat to reduce curing time from hours to minutes with minimal external energy. Combining exothermic heat with press molding, the novel EPFP enables the efficient fabrication of complex geometries, such as airfoil skin sections, with high fiber volume fractions (above 60%). In addition, EPFP is compatible with commercial off‐the‐shelf epoxy by integrating frontal resin, showcasing its versatility and adaptability for diverse industrial applications. Composites manufactured using EPFP exhibit superior thermomechanical properties while significantly reducing energy consumption by 80% and production costs by 40%. This makes it a sustainable and efficient solution for polymer composites manufacturing. 

Abstract Nanocomposites containing nanoscale materials offer exciting opportunities to encode nanoscale features into macroscale dimensions, which produces unprecedented impact in material design and application. However, conventional methods cannot process nanocomposites with a high particle loading, as well as nanocomposites with the ability to be tailored at multiple scales. A composite architected mesoscale process strategy that brings particle loading nanoscale materials combined with multiscale features including nanoscale manipulation, mesoscale architecture, and macroscale formation to create spatially programmed nanocomposites with high particle loading and multiscale tailorability is reported. The process features a low‐shrinking (<10%) “green‐to‐brown” transformation, making a near‐geometric replica of the 3D design to produce a “brown” part with full nanomaterials to allow further matrix infill. This demonstration includes additively manufactured carbon nanocomposites containing carbon nanotubes (CNTs) and thermoset epoxy, leading to multiscale CNTs tailorability, performance improvement, and 3D complex geometry feasibility. The process can produce nanomaterial‐assembled architectures with 3D geometry and multiscale features and can incorporate a wide range of matrix materials, such as polymers, metals, and ceramics, to fabricate nanocomposites for new device structures and applications.