Applications such as batteries, fuel cells, solar cells, and sensors, can benefit from high surface-to-volume ratio core/shell arrays of nanorods. The fabrication of the conformal shell layers on nanorod arrays has been a formidable task. In order to assess the deposition conditions for the production of conformal shell coatings by physical vapor deposition (PVD) techniques, we employed Monte Carlo (MC) simulations that involved shell depositions under different flux distributions and angles on arrays of rods. We investigated the conformality of PVD shell layers on nanorod arrays of different aspect ratios, which is defined to be the ratio of rod height to the gaps between nearest-neighbor rods. MC simulated core/shell structures were analyzed for the thickness uniformity of the shell layer across the sidewalls of rods. Our results show that a small angle deposition approach involving a uniform oblique flux (U-SAD) with a small incidence angle ≤ 30o can generate a fairly conformal shell coating around small aspect-ratio rods. However, normal angle deposition with an angular flux distribution (A-NAD) achieves superior conformality both on small and high-aspect-ratio structures compared to U-SAD, conventional uniform normal angle deposition (U-NAD), and SAD with an angular flux distribution (A-SAD). A-NAD can be realized in a PVD system such as by high pressure sputter deposition; while U-SAD can be achieved in thermal evaporation system with a small angle incident flux. In addition, U-NAD and A-SAD can correspond to film growth by normal incidence thermal evaporation and SAD-high pressure sputter deposition, respectively.