Modification of CNF‐Networks by the Addition of Small Amounts of Well‐Defined Rigid Cationic Nanolatexes

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Cellulose nanofibril (CNF)‐networks are modified by the addition of small amounts (below 10 wt%) of well‐defined cationic nanolatexes synthesized through reversible addition–fragmentation chain‐transfer‐mediated polymerization‐induced self‐assembly (PISA). Minute amounts of nanolatex inclusions lead to increased tensile and shear moduli, indicating that nanolatexes can act as bridging‐points between CNFs. At higher nanolatex content, this stiffening effect is lost, likely due to interactions between nanolatexes leading to plasticization. The influence of nanolatex content and size on interparticle distance is discussed and is used as a tool to understand the effects observed in macroscopic properties. Upon annealing, the stiffening effect is lost due to the softening of the nanolatexes, indicating that the core–shell morphology is a prerequisite for this effect. These systems form a versatile platform to develop fundamental insights into complex condensed colloidal systems, to ultimately aid in the development of new sustainable material concepts.