▎ 摘　　要

Hydrogenation is a viable approach in transforming two-dimensional (2D) nanosheets into three-dimensional (3D) nanoarchitectures. The present work reported self-folding of 2D graphene into 3D graphene Miura origami assisted by hydrogenation, and studied its Poisson's ratio under external strain using molecular dynamics simulation and continuum modeling. It was found that the graphene Miura origami possesses negative Poisson's ratio, being largely insensitive to the chirality of the folding creases and side lengths of the constituting parallelograms. We further demonstrated the good agreement of Poisson's ratio between the continuum prediction and MD simulation, and identified the origin of their deviation as localized stress concentration at the quad-junction of the graphene Miura origami. The present study provides insights into designing novel 3D nanoarchitectures of programmable functionalities from 2D nanomaterials.