||Anode materials undergo intercalation mechanism are considered to provide stable electrochemical sodium storage for SIB applications. Though MoS2 is a promising 2D material for SIBs, it suffers from deformation of layered structure during repeated intercalation of Na+, resulting in undesirable electrochemical behaviors. In this study, vertically oriented MoS2 on nitrogenous reduced graphene oxide sheets is presented with designed spatial geometries, which can deliver a remarkably high reversible capacity of 255 mA h g−1 at a current density of 0.2 A g−1 and 245 mA h g−1 at a current density of 1 A g−1, with a total fluctuation of 5.35% over 1300 cycles. These results are superior to those obtained with hard carbon structures. Furthermore, a SIB full cell composed of the optimized anode and a Na2V3(PO4)3 cathode reaches a specific capacity of 262 mA h g−1 during 50 cycles, with an operated voltage range of 2.4 V, demonstrating the potentially rewarding SIB performance.