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Lignin nanoparticles (LNPs), as one of green and sustainable biological macromolecules, have attracted great attention owing to their promising potentials in many valorized fields. However, the lignin heterogeneity seriously restricts the controllable preparation of LNPs. Herein, a facile nanogrinding activation combining anhydrous ethanol dissolution process was developed to efficiently homogenize lignin prior to gradient ethanol fractionation. Two lignin fractions were obtained from nanogrinding activation/ethanol dissolution followed by gradient ethanol fractionation: L-fractions and S-fractions. Therefore, monodispersed LNPs with unique concave hollow nanostructure and large particle size, and monodispersed LNPs with solid core nanostructure and small particle size were successfully prepared from L-fractions and S-fractions, respectively, via a GVL/water anti-solvent method. The proposed LNPs formation mechanisms facilitated by nanogrinding activation/ethanol dissolution treatment were demonstrated. This study put forwards a facile and green integrated approach for monodispersed LNPs preparation with controllable morphology and particle size. [Display omitted] • Nanogrinding/ethanol treatment facilitates lignin cleavage and fractionation. • The synergistic effect fractionates lignin into L- and S- fractions. • L-/S-fractions possess unique functional groups and molecular distributions. • Monodispersed LNPs with concave hollow and core nanostructures are prepared. • The proposed mechanisms of LNPs formation are demonstrated. [ABSTRACT FROM AUTHOR]