The programmable nature of graphene kirigami enables it highly applicable in the development of stretchable nanodevices. In this study, we employed molecular dynamics simulations to investigate the large deformation behavior of a structured graphene kirigami nano-spring (GKNS) with re-entrant honeycombs. During a uniaxial test, the elastic deformation can be categorized into two stages based on the applied load level. Stage I exhibits a maximal strain (εYstart) exceeding 50 % under low loading conditions, while stage II demonstrates a strain (εYend) surpassing 70 % at a high hardening rate. Both εYstart and εYend are greater than those observed in GKNS with transversal periodic boundary conditions. Furthermore, increasing the length or decreasing the width of bars within GKNS with cells of identical shape leads to an increase in both εYstart and εYend values. Ambient temperature has minimal impact on εYstart and εYend however, higher temperatures result in lower hardening rates due to weakened carbon–carbon bonds within GKNS structures. Additionally, variations in cell/void arrangement within structured GKNS affect both εYstart and εYend values, whereas widening the GKNS structure leads to reduced hardening rates. The findings presented herein provide valuable insights for designing nanodevices that necessitate significant deformations.