The search for sustainable material solutions has put lignin as one of the prime candidates for aromatic building blocks in macromolecular materials. The present study aimed to demonstrate how lignin-based thermoset resins can be utilized in combination with different cross-linkers. Kraft lignin was used to produce thermosets with tunable mechanical and morphological properties. The lignin-based thermosets were obtained via a thermally induced thiol–ene reaction. The first part of this work was focused on Kraft lignin solvent fractionation and chemical modification of the ethanol soluble fraction. Chemical analysis indicated that the allylation process was selective toward phenolic hydroxyl groups. SAXS and SEM studies demonstrated that sol...