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Formation mechanism of ledeburites in laser alloying composite coating on a titanium alloy was investigated. The amorphous reinforced composite coatings were fabricated on the TA2 alloys by laser alloying of Co-Al-Fe-TiC/C mixed powders. Through the X-ray diffraction and high resolution transmission electron microscope test, it was confirmed that the amorphous phases were produced in such a coating. Scanning electron microscope results indicated that the ledeburites were produced in the Co-Al-Fe-C laser alloying coating, and the content of the ceramics played an important role in the formation mechanism of ledeburites. This research provides essential experimental basis to promote the application of laser alloying technique in the surface modifications of the titanium alloys.