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Steels inevitably suffer friction and corrosion during service, often decreasing durability and functionality. This work presents a novel silane-based composite film that exhibits robust corrosion resistance. When deposited on steels, these films demonstrate exceptional anti-corrosion properties with a high impedance value, even when exposed to highly corrosive media for extended periods (e.g., 240 h). Furthermore, the films show minimal morphological damage after a long-term stability experiment of 25 days in a 3.5 wt % NaCl solution, compared with bare 304 stainless steels (SS). Theoretical studies have been conducted to elucidate the corrosion resistance and sol-gel mechanisms. Upon lubrication, the universal micro-tribotester (UMT) results demonstrate that friction decreases with applied load. The lowest friction coefficient (COF) value of 0.14 is achieved at a regular load of 1 N and a sliding velocity of 0.1 mm/s. The COF performances of these films are explained based on their hydrophobic/hydrophilic nature, uniformity, and Raman spectrum. The Raman spectrum indicates that the excellent friction properties at the sliding interface are attributed to fullerol. This process will inspire a robust, low-cost, and environmentally friendly approach to protecting steel. [Display omitted] • New silane/fullerol/α-SiC films were fabricated using a facile brushing process. • Long-term tribo-corrosion resistance performance were significantly improved. • Computational simulations revealed mechanisms of molecular interactions. [ABSTRACT FROM AUTHOR]