Polyaniline nanofibers (PANI NFs) are introduced to construct a wind-driven triboelectric nanogenerator (TENG) as a new power source for self-powered cathodic protection. PANI NFs serve as a friction layer to generate charges by harvesting wind energy as well as a conducting layer to transfer charges in TENG. A PANI NFs-based TENG exhibits a high output performance with a maximum output voltage of 375 V, short current circuit of 248 μA, and corresponding power of 14.5 mW under a wind speed of 15 m/s. Additionally, a self-powered anticorrosion system is constructed by using a PANI-based TENG as the power source. The immersion experiment and electrochemical measurements demonstrate that carbon steel coupled with the wind-driven TENG is effectively protected with an evident open circuit potential drop and negative shift in the corrosion potential. The smart self-powered device is promising in terms of applications to protect metals from corrosion by utilizing wind energy in ambient conditions.