Melanin-like nanoparticles (MLNPs) hold great promise for biomedical applications, yet their controlled synthesis under mild conditions remains challenging. Here, we present a hydrogen bond-mediated liquid-liquid phase separation (LLPS) strategy to fabricate functional MLNPs with tunable physicochemical properties. Coacervates are formed through hydrogen bonding between hydrogen bond donor polyphenols and hydrogen bond acceptor polymers, providing a dynamic and mild environment for nanostructure formation. Leveraging this hydrogen bond-stabilized coacervate as a soft template, we synthesized monodisperse MLNPs via oxidative polymerization of coacervates. The resulting nanoparticles feature precise size control and abundant surface functionalities, enabling drug loading via electrostatic interactions, hydrogen bonding, pi-pi stacking, and metal-ion coordination. These multifunctional properties support diverse biomedical applications, including drug delivery, imaging, and enzyme-mimetic catalytic therapy. This work establishes a scalable and versatile platform for engineering MLNPs via hydrogen bond-driven LLPS templating, opening up opportunities for translational nanomedicine.
[1]Shandong Univ, Sch Chem & Chem Engn, Key Lab Colloid & Interface Chem, Minist Educ, Jinan 250100, Shandong, Peoples R China.
[2]Shandong Key Laboratory of Magnetic FieldFree Medicine & Functional Imaging, Research Institute of Magnetic Field-Free Medicine & Functional Imaging,National Medicine-Engineering Interdisciplinary IndustryEducation Integration Innovation Platform, Qilu Hospital of Shandong University, Jinan, Shandong 250012, China
[3]Email: zlgao@email.sdu.edu.cn
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