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A series of chemical cross-linked nanoporous cellulose hydrogels (CCNCGs) were prepared, and their fracture strain increased first and then decreased as the molar ratio of epichlorohydrin (ECH) to the anhydroglucose unit (AGU) of cellulose increased. Two polymer matrices, polycaprolactone (PCL) and polyurethane (PU), were selected to be polymerized in CCNCGs in situ. The fracture strain of CCNCG/PCL and CCNCG/PU nanocomposites in the tensile test showed the same tendency as neat CCNCGs in the hydrated state, regardless of the surroundin