It is demonstrated that 3D nanostructured polypyrrole (3D PPy) nanocomposites can be reinforced with PPy covered nanocellulose (PPy@nanocellulose) fibres to yield freestanding, mechanically strong and porosity optimised electrodes with large surface areas. Such PPy@nanocellulose reinforced 3D PPy materials can be employed as free-standing paper-like electrodes in symmetric energy storage devices exhibiting cell capacitances of 46 F g(-1), corresponding to specific electrode capacitances of up to ∼185 F g(-1) based on the weight of the electrode, and 5.5 F cm(-2) at a current density of 2 mA cm(-2). After 3000 charge/discharge cycles at 30 mA cm(-2), the reinforced 3D PPy electrode material also showed a cell capacitance corresponding to 92% of that initially obtained. The present findings open up new possibilities for the fabrication of high performance, low-cost and environmentally friendly energy-storage devices based on nanostructured paper-like materials.