Nowadays, the development of sustainable high-performance functional nanomaterials is in the spotlight. In this work, we report the preparation of a new generation of flexible and high electroconductive nanopapers based on nanofibrillated cellulose (NFC) and copper nanowires (CuNWs). Homogeneous red brick color nanopapers (thickness 30.2–36.4 μm) were obtained by mixing different amounts of NFC aqueous suspensions and CuNWs (1, 5, 10, 20, and 50 wt %), followed by vacuum filtration and drying. scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS) analysis confirmed the incorporation of the different amounts of CuNWs, and their uniform and random distribution. All of the nanomaterials displayed good mechanical properties, viz., Young’s modulus = 2.62–4.72 GPa, tensile strength = 30.2–70.6 MPa, and elongation at break = 2.3–4.1% for the nanopapers with 50 and 1 wt % of CuNWs mass fraction, respectively. The electrical conductivity of these materials strongly depends on the CuNW content, attaining a value of 5.43 × 104 S·m–1 for the nanopaper with a higher mass fraction. This is one of the highest values reported so far for nanocellulose-based conductive materials. Therefore, these nanopapers can be seen as an excellent inexpensive and green alternative to the current electroconductive materials for applications in electronic devices, energy storage, or sensors.