A serious of CrN/AlTiN nanolaminate films with different deposition temperatures were synthesized by Multi-Arc-Ion Plating (MAIP). The composition and microstructural evolution, hydrophobicity, and mechanical properties of CrN/AlTiN nanolaminate films were studied. It was found that these films were structured by FCC metal nitride phases and the preferred orientation changed form (111) to (200) with the deposition temperature increased to 450 °C. The SEM and TEM results showed that the rate of deposition as well as modulation period increased as the deposition temperature increased. On the contrary, the amount of macroparticles on the film's surface and the Cr content [Cr/(Cr + Ti + Al) ratio] decreased as the temperature increased. Among these films, CrN/AlTiN nanolaminate films deposited at 450 °C exhibited the highest hardness (∼37 GPa), lowest coefficient of friction (0.17). The contact angle (CA) results showed that the CrN/AlTiN nanolaminate composites films were hydrophobic and could be superhydrophobic after modification, which provided a new insight to prepare robust superhydrophobic films.