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Hydrophilic and LCST polymer chains, poly(N,N-dimethylacrylamide) (PDMA) andpoly(Nisopropylacrylamide)(PNIPA), were combined in semi-interpenetratedarchitectures toinvestigate their responsive properties in swollen isochoricconditions comparatively tografted network structures. Using equal weightfractions of PDMA and PNIPA, semi-IPNdesigned with opposite topologies havedemonstrated a thermoresponsive behavior with verydifferentstructure/properties relationships as investigated by calorimetry,swellingexperiments, tensile tests and 2D neutron scattering at rest and underdeformation. In the caseof the PDMA network interpenetrated by linear PNIPAchains, the phase transition of PNIPAgives rise to the formation of largemicrodomains, loosely percolating the PDMA network.Above the transition, theenhancement of the mechanical properties remains low in terms ofelastic modulusand fracture energy. Conversely, the opposite topology, with PDMAchainsinterpenetrating the crosslinked PNIPA network, brings a largeimprovement of themechanical properties at high temperature with a 10-foldincrease of the modulus and veryhigh fracture energy. By comparison withgrafted hydrogels of similar composition anddifferent topologies, the impact ofthe primary structure over the phase-separated morphologyand the resultingmechanical properties was clearly highlighted.

Thermoresponsive Toughening in LCST-Type Hydrogels: Comparison between Semi-Interpenetrated and Grafted Networks