Titanium alloys are often used in engineering fields including aerospace, cryogenic technologies, and weaponry due to their remarkable qualities. However, several issues including a high coefficient of friction, weak wear resistance, and low hardness hinder their widespread usage. Despite several efforts to enhance their tribology, achieving ultra-low friction on titanium alloy surfaces remains a challenging problem in materials science. Here, we report on the superlubricity of a MoS2 + a-C:H (Mo-a films) composite film, prepared by magnetron sputtering and spraying to lubricate titanium alloy surfaces. Robust superlubricity was achieved by the Mo-a composite films with a coefficient of friction (COF) below 0.007 in a helium environment. Compared to the reference titanium alloy substrates, the introduction of Mo-a composite film reduced the friction coefficient to roughly 1%, and the a-C:H film reduced wear by three orders of magnitude. High-resolution characterizations indicate that this enhanced tribology can be attributed to the formation of transfer film, which is enriched with nanostructured graphene sheets and MoS2 nanoscrolls, and is formed due to shear stress-induced structural transformation of a-C:H films and MoS2 nanosheets. This transfer film transitioned the initial high-resistance steel-to-a-C:H contact to super low-resistance steel-to-transfer film contact, thus achieving superlubricity and a remarkable wear reduction. This work outlines a pathway to solving the poor wear resistance and high friction coefficient problem of titanium alloy surfaces, which can be an important guideline for applications of titanium alloys in mechanical engineering.