In this article the diamond-like carbon films have been prepared by the strategy of the glancing angle deposition using unbalanced magnetron sputtering technique. It is found that the structure and the residual stress of the films are strongly dependent on the deposition angle. Of particular interest is that the stress of the films significantly transforms from compressive to tensile state as a function of the deposition angle, which is attributed to the result of the competition and mediation between compressive stress due to surface capillary forces of the island surface and tensile stress due to the coalescence of the islands during Volmer-Weber growth of the films. Based on this mechanism, the nearly stress-free film with desirable performance can be prepared at the proper deposition angle. The correlation between the residual stress and the atomic-bond structure also reveals that the stress transition is not only related to the sp(2)-bonded carbon content, but also closely to the changes of the heptatomic and pentatonic rings in the carbon network. This work demonstrated herein will provide a promising route to prepare the stress-free diamond-like carbon films with desirable performance.