Diamond-like carbon (DLC) films, deposited by dry processes, such as, physical vapor deposition and chemical vapor deposition, provide high hardness, lubricity, and wear resistance. With improvements in microfabrication technologies, tuning the microscopic surface morphology to control physical properties (such as wettability) of materials has attracted immense attention. However, the strengths of microstructures with uneven surfaces are insufficient for numerous applications. Therefore, nanoscale structures with uneven surfaces and enhanced strength were synthesized using DLC. Anodic porous alumina films with regularly aligned linear nanopores produced by anodic oxidation of Al were used as mask materials to deposit DLC films on Si substrates. Uneven structures (with uniform distributions of DLC nanoscale protrusions) were created on the substrates. Mask materials with large pore diameters and small thicknesses created DLC protrusions with large diameters and heights, respectively. The friction coefficients of nanostructured DLC surfaces with tall protrusions and normal DLC films were similar. Unevenly structured DLC surfaces were slightly more water-repellent than normal DLC films, with greater water repellency for taller protrusions. The Cassie-Baxter model was applied to analyze the surface wettability. This report describes a new, simple, and effective method of fabricating DLC nanoscale structures using anodic alumina films.