The growing demand for sustainable products has spurred research into renewable materials, with cellulose-based materials emerging as prominent candidates due to their exceptional properties, abundance, and wide-ranging applications. In this context, there is a need to develop a better fundamental understanding of cellulose interactions such that we can continue to design and improve sustainable materials. Individual interactions can be difficult to assess in bulk fibre-based materials and therefore cellulose model materials have become indispensable tools for researchers as they can facilitate the study of cellulose interactions at a molecular level enabling the design of sustainable materials with enhanced properties. This study presents a new methodology for studying the effects of surface treatments on the individual fibre–fibre joint strength using wet-spun cellulose nanofiber (CNF) filaments as model materials. The Layer-by-Layer assembly technique is used to modify the surface chemistry of the model materials as well as bleached and unbleached hardwood Kraft fibres, demonstrating its potential to enhance adhesive properties and overall mechanical performance of papers made from these fibres. The study further explores the impact of increasing network density through wet-pressing during paper preparation, showcasing a comprehensive approach to molecularly tailor fibre-based materials to achieve superior mechanical properties. The proposed methodology provides a time-efficient evaluation of chemical additives in paper preparation.