Rational design of electrode materials for sodium-ion batteries with high flexibility is still challenging. Here, superelastic 3D few-layer MoS2/carbon framework heterogeneous electrodes (abbreviated as, MoS2@CF) are fabricated by a simple vacuum infiltration and heating process. The interconnected ultrathin MoS2 network filled with carbon framework forms a 3D heterogeneous network with hierarchical pore structure. The unique structure of the electrodes results in excellent mechanical and electrochemical performances. The MoS2@CF electrodes exhibit superior elasticity and recoverability. After 180° bending repeatedly, the electrodes still can recover their initial sizes. Moreover, the electrodes show outstanding cycling stabilities with high reversible capacities reaching up 240 mA h g−1 after 500 cycles at 1 A g−1 (capacity retention of ~ 99%). Full-cells assembled with MoS2@CF anodes and Na3V2(PO4)3 cathodes show high reversible capacity (~ 252 mA h g−1 at 0.5 A g−1). Overall, the superior mechanical properties and high electrochemical performances indicate the promising potential of MoS2@CF electrodes in large-scale flexible sodium-ion storage devices.