Lignin nanoparticles (LNPs) have been showing great potential for multiple applications in recent years. To further develop such nano polymer to satisfy the needs of industries, rational synthesis methods are prerequisites for controlling structures and morphologies of LNPs. In this study, we aimed to understand the lignin self-assembly kinetics based on the population balance theory. The self-assembly of lignin toward nanoparticles can be explained by the particle-particle interaction energy based on the assumption that a lignin single chain can act as a single particle. As the growth of LNPs is determined by the balance between attractive force (<i>i.e.,</i> van der Waals force) and repulsion force (<i>i.e.,</i> electrostatic repulsive force by lignin’s inherent phenolic and carboxylic groups), the rationally developed population balance kinetic model combined with the colloidal forces between LNPs can predict the nanoparticle sizes. Based on the developed model, we elucidated that the LNPs’ sizes can be determined by the amount of the ionized groups on the nanoparticles and their ionic equilibrium factors according to the electrolyte and pH condition of the antisolvent via coupling of the theoretical studies and experimental validations. Our findings would support the wide-applicable and controllable LNP production process, along with the high flexibility of LNP in various application fields.

Mechanistic understanding of lignin self-assembly with controlled nanoparticle sizes

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