Laser 3D printing, also known as laser additive manufacturing (LAM), is favored for its ability to form bulk metallic glass (BMG) and its composite materials (BMGcs) with freeform geometries. In this work, two different kinds of Fe41Co7Cr15Mo14C15B6Y2 amorphous coatings (A and B) were prepared by using LAM technology under air- and water-cooled conditions, respectively; meanwhile, to reduce the cracks generated due to the residual thermal stresses, coating C obtained by air-sweep annealing of B with a low energy-density laser. The morphology and amorphous content and microstructure of the coatings were investigated, the results show many cracks in coating B deposited under water-cooled conditions, and its microstructure shows an amorphous-crystal-nanocrystalline mixed structure. Cracking was suppressed in coating C, obtained by air-sweep annealing based on coating B, but the amorphous content was reduced from 32.6 to 13.4%. And the hardness and corrosion resistance of the coating will increase with the increase in the amorphous content. Finally, the internal friction behavior of a BMGcs was prepared on the basis of the process of sample C is compared with that of as-cast amorphous alloys. The results show that the low temperature internal friction behavior of BMGcs is affected by the defects produced during printing, and the high temperature internal friction behavior is affected by the precipitated hard phase.