To circumvent elaborate conventional lithographic methods for realizing metallic nanostructures, it is necessary to develop self-organized nanofabrication methods for suitable template structures and their optical characterization. We demonstrate the potential of ion bombardment with impurity co-deposition to fabricate terraced or quasi-blazed nanostructure templates. Self-organized terraced nanostructures on fused silica were fabricated using
A
r
+
ion bombardment with iron impurity co-deposition and subsequent Au shadow deposition. The aspect ratios are enhanced threefold, and the range of nanostructure period variation is significantly increased with respect to that of conventional nanostructures realized by pure ion bombardment. We reveal the key features of the method via atomic force microscopy and optical characterization. Variable-profile quasiperiodic nanostructures with periods of 100–450 nm, heights of 25–180 nm, and blaze angles of 10°–25° were fabricated over an area of
20
×
40
m
m
2
, and these exhibited tunable and broadening optical anisotropy across the nanostructured area. Thus, the proposed method is a viable technique for rapid, cost-effective, and deterministic fabrication of variable nanostructure templates for potential optical applications.