Designing yield stress fluids to exhibit desired functional
properties
is an integral challenge in many applications such as 3D printing,
drilling, food formulation, fiber spinning, adhesives, and injectable
biomaterials. Extensibility in particular has been found to be a highly
beneficial characteristic for materials in these applications; however,
few highly extensible, high water content materials have been reported
to date. Herein we engineer a class of high water content nanocomposite
hydrogel materials leveraging multivalent, noncovalent, polymer–nanoparticle
(PNP) interactions between modified cellulose polymers and biodegradable
nanoparticles. We show that modulation of the chemical composition
of the PNP hydrogels controls the dynamic cross-linking interactions
within the polymer network and directly impacts yielding and viscoelastic
responses. These materials can be engineered to stretch up to 2000%
strain and occupy an unprecedented property regime for extensible
yield stress fluids. Moreover, a dimensional analysis of the relationships
between extensibility and the relaxation and recovery time scales
of these nanocomposite hydrogels uncovers generalizable design criteria
that will be critical for future development of extensible materials.