Abstract Inflammatory diseases (IDs), characterized by chronic inflammation and symptoms including redness, swelling, heat, and pain, present substantial global health and economic burdens. Conventional anti‐inflammatory therapeutic strategies often offer only temporary relief, and fail to achieve targeted, sustained, and safe modulation of the inflammatory microenvironment. Peptide‐based materials (PBMs) have emerged as a highly promising platform for precision inflammation modulation, leveraging their inherent biocompatibility, tunable structures, and capacity for self‐assembly into diverse supramolecular architectures. This review systematically categorizes these PBMs into self‐assembling peptides, conjugated peptide assemblies, and coassembled systems, delineating their design principles, assembly mechanisms, inflammation reprogramming and immunomodulation functions. Recent advances in their application for IDs treatment are critically evaluated and emerging strategies are introduced, notably the integration of artificial intelligence in peptide design. Finally, current translational challenges are discussed and perspectives on future research directions and clinical potential are provided.