The need for renewable alternatives for fossil-based aromatic material constituents is evident for a more sustainable society. Lignin is the largest source of naturally occurring aromatic compounds but has mainly been considered as waste material or energy source in the pulp and paper industry. Developments in extracting lignin from these processes provide a large source for renewable aromatic structures to be used in various applications. Producing thermosets out of lignin is a very promising route to utilize this raw material toward, for example, composite application. The buildup of the molecular network based on oligomeric lignin segments will be different from traditional thermoset analogues, where the constituents often are smaller molecules, and will have an effect on the material properties. In this work LignoBoost Kraft lignin is refined, chemically modified, and used to produce freestanding thermosets with different architectures and properties. These different thermosets are evaluated, and the possibilities to tailor the material properties through work-up and modification are demonstrated. Morphological studies on the formed thermosets using X-ray scattering show systematic differences in molecular stacking and aggregate sizes.