Transition-metal oxides (TMOs) are considered as promising anode materials for lithium ion batteries. However, the poor structural stability and relatively low electronic conductivity greatly limit their application in flexible electronic devices. Herein, a 3D hierarchical high performance MnO-based flexible electrode is fabricated through vacuum-assisted layer-by-layer assembly of 1D polydopamine coated MnO2 nanowires (MnO2@PDA NWs) and 2D graphene oxide nanosheets (GO NSs), followed by a thermal reduction process. The resulting composite (MnO@C-rGO) demonstrates excellent flexibility, structure stability and manifests outstanding lithium storage performance in terms of high reversible capacity (920 mAh g−1 at 0.2 A g−1), excellent rate capability (686 mAh g−1 at 2 A g−1 and 396 mAh g−1 at 10 A g−1) and impressive cycling stability (719 mAh g−1 at 2 A g−1 without fading after 800 cycles), exceeding most of recently reported MnO-based anodes. It is proved that the freestanding flexible MnO@C-rGO anode can be successfully applied in flexible full cell, which achieves superior flexibility and maintains good electrochemical performance during mechanical deformations.