Carboxymethyl cellulose modified with norbornene groups (NorCMC) and cellulose nanofibrils (CNFs) produced through mechanical refining without chemical pretreatment formed interpenetrating network hydrogels through a UV-light initiated thiol-ene reaction. The molar ratio of thiols in crosslinkers to norbornene groups off the NorCMC (T:N), total polymer weight percent in the hydrogel, and weight percent of CNFs of the total polymer content of the hydrogels were varied to control hydrogel properties. This method enabled orders of magnitude changes to behavior. Swelling in aqueous environments could be significant (>150 %) without CNFs to minimal (<15 %) with the use of 50 % CNFs. NorCMC and CNF networks interacted synergistically to create hydrogels with compression modulus values spanning 1 to 150 kPa - the values of most biological tissues. T:N and total polymer weight percent could be varied to create hydrogels with different CNF content, but the same compression modulus, targeting 10 and 100 kPa hydrogels and providing a system that can independently vary fibrillar content and bulk modulus. Analysis of the effective crosslinks, thiol-ene network mesh size, and burst release of the polymer indicated synergistic interactions of the NorCMC thiol-ene and CNFs networks. These interactions enhanced modulus and degradation control of the network under physiological conditions.
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