Most synthetic materials,when subjected to dynamic stress,will undergo microstructural damage.Conversely,biological tissues could alter the internal and external configuration through adaptation to these stresses.Graphene oxide(GO)paper subjected to low-amplitude dynamic tension has shown a self-stiffening response previously unobserved in nanostructured carbon materials based macrospcopic architectures.In addition,there is an as high as 200%increase in Youngs Modulus for GO paper after dynamic process.We further defined a model to analyze the structure-property relations during stiffening process.Systematic mechanical test,characterizations and molecular dynamics simulations have proved that the parameters in our model could quantitatively evaluate the morphology of microstructure and the ability of reorientation of sheets in GO papers.Our model could also incorporate mechanical behaviors of both GO sheets and their interaction for a full understanding of overall mechanical properties of graphene-based paper materials and further guide rational design of self-stiffening functional materials.These results are believed to be of help to harness the strain hardening mechanisms and could be useful for the development of biocompatible and adaptable structural materials for biomechanical tissues replacement.