In this paper, we propose an efficient and effective method to fabricate highly ordered Cr nanoarrays with sub-gaps less than 15 nm and particle size less than 50 nm on the top surface of a modified porous anodic alumina membrane (PAA). In addition, the factors that influence the structural parameters of the fabricated nanostructures were studied. With the aid of SEM and AFM images, the amount of sputter-coated Cr was tailored to the given PAA surface morphology. The mechanism of formation of the Cr nanostructures was also discussed.