The doping of amorphous carbon is one way of specifically modifying its properties. The present work is a contribution to understand the effect of dopant selection on structure, mechanical properties and crack resistance of hydrogen-free tetrahedral amorphous carbon (ta-C) coatings. For this purpose, nonmetallic (B, Si) and metallic (Mo, Fe, Cu) dopants were selected. The coatings were produced by the Laser-Arc technique and investigated by Raman spectroscopy, transmission electron microscopy, nanoindentation, bending, and scratch tests. It was found that doping generally affected the sp² content and cluster size of the sp² carbon phase, and thus hardness, Young's modulus, and intrinsic compressive stresses, but also the defect content and the crack resistance. The addition of metallic dopants led to an increase and clustering of the sp²-bonded carbon and, consequently, to a significant reduction in hardness and Young's modulus. This effect was much less pronounced when doping with non-metallic elements. The failure behavior changed toward higher ductility and crack resistance when metals were added. The crack resistance was found to be directly dependent on the H³/E² value, with H³/E² > 0.2 leading to a more brittle behavior with unstable crack propagation, while at H³/E² < 0.2 the material was more ductile and exhibited stable crack propagation and thus higher crack resistance.