This study explores the influence of process parameters on the structural, mechanical, and electrical properties of ZrAlNiCu alloy and nitride film obtained by magnetron sputtering of a single Zr51Al11Ni4Cu34 target. Selected variables affecting the process are working pressure, substrate temperature, and nitrogen partial pressure. Almost all films are amorphous except for nitride films deposited at moderate nitrogen partial pressure, which consist of the FCC-ZrN nanophase. A low working pressure and high substrate temperature result in refined boundary interfaces, thus increasing their hardness and electrical conductivity. Nitride films have higher hardness and lower electrical conductivity than alloy films because of their strong ionic metal-N bonding. Thus, the formation of FCC-ZrN nanocrystals is conducive to the further improvement of hardness.