Abstract
The two-dimensional structure of graphene makes it difficult to realize flexibility and auxeticity (negative Poisson's ratio) in graphene-based structures. Using molecular dynamics simulations, we demonstrate for graphene origami structures effective tuning of both the flexibility and Poisson's ratio through the geometry, including the potential to combine superflexibility with a highly tunable negative Poisson's ratio in contrast to any existing graphene-based structure. Auxeticity even can be achieved under large applied strain, both tensile and compressive.