The growing adoption of biobased materials for electronic, energy conversion, and storage devices has relied on high-grade or refined cellulosic compositions. Herein, lignocellulose nanofibrils (LCNF), obtained from simple mechanical fibrillation of wood, are proposed as a source of continuous carbon microfibers obtained by wet spinning followed by single-step carbonization at 900 °C. The high lignin content of LCNF (∼28% based on dry mass), similar to that of the original wood, allowed the synthesis of carbon microfibers with a high carbon yield (29%) and electrical conductivity (66 S cm^–1). The incorporation of anionic cellulose nanofibrils (TOCNF) enhanced the spinnability and the porous morphology of the carbon microfibers, making them suitable platforms for electrochemical double layer capacitance (EDLC). The increased loading of LCNF in the spinning dope resulted in carbon microfibers of enhanced carbon yield and conductivity. Meanwhile, TOCNF influenced the pore evolution and specific surface area after carbonization, which significantly improved the electrochemical double layer capacitance. When the carbon microfibers were directly applied as fiber-shaped supercapacitors (25 F cm^–3), they displayed a remarkably long-term electrochemical stability (>93% of the initial capacitance after 10 000 cycles). Solid-state symmetric fiber supercapacitors were assembled using a PVA/H₂SO₄ gel electrolyte and resulted in an energy and power density of 0.25 mW h cm^–3 and 65.1 mW cm^–3, respectively. Overall, the results indicate a green and facile route to convert wood into carbon microfibers suitable for integration in wearables and energy storage devices and for potential applications in the field of bioelectronics.