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Layered double hydroxides (LDHs) have demonstrated excellent tribological performance in various studies. However, there remains a fundamental knowledge gap concerning the chemical composition of tribofilms across the cross-section. In this study, we seek to elucidate this question by tribologically testing various binary LDHs. It was found that five out of eight LDHs, denoted as CoAl-, CoFe-, MgAl-, NiFe-, and ZnAl-LDHs could induce hierarchical protective tribofilms due to the formation of rigid oxide layers and in situ carbon-based films. The five tribofilms helped to reduce wear loss and friction by approximately 90% and 20%, respectively. Remarkably, the Co-based tribofilms showed the best antiwear performance because of the thick carbon tribofilm formation and the strong bonding at the metallic/tribo-oxide interfaces. The formation mechanisms of the carbon tribofilm and its characteristic nature were evaluated and revealed by scanning transmission electron microscopy and electron ....