Most of immunomodulatory materials (e.g., vaccine adjuvants such as alum) modulate adap-tive immunity, and yet little effort has focused on developing materials to regulate innate im-munity, which get mentioned only when inflammation affects the biocompatibility of bio-materials. Traditionally considered as short-lived effector cells from innate immunity primarily for the clearance of invading microorganisms without specificity, neutrophils exhibit key role in launching and shaping the immune response. Here we show that the incorporation of un-natural amino acids into a well-known chemoattractant-N-formyl-L-methionyl-L-leucyl-L-phenylalanine (fMLF)-offers a facile approach to create a de novo, multifunctional chemoat-tractant that self-assembles to form supramolecular nanofibrils and hydrogels. This de novo chemoattractant not only exhibits preserved cross-species chemoattractant activity to human and murine neutrophils, but also effectively resists proteolysis. Thus, its hydrogel, in vivo, re-leases the chemoattractant and attracts neutrophils to the desired location in a sustainable manner. As a novel and general approach to generate a new class of biomaterials for modu-lating innate immunity, this work offers a prolonged acute inflammation model for developing various new applications.
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