Contact lenses are ubiquitous biomedical devices used for vision correction and cosmetic purposes. Their application as quantitative analytical devices is highly promising for point-of-care diagnostics. However, it is a challenge to integrate nanoscale features into commercial contact lenses for application in low-cost biosensors. A neodymium-doped yttrium aluminum garnet (Nd:YAG) laser (1064 nm, 3 ns pulse, 240 mJ) in holographic interference patterning mode was utilized to produce optical nanostructures over the surface of a hydrogel contact lens. One-dimensional (925 nm) and two-dimensional (925 nm × 925 nm) nanostructures were produced on contact lenses and analyzed by spectroscopy and angle-resolve measurements. The holographic properties of these nanostructures were tested in ambient moisture, fully hydrated, and artificial tear conditions. The measurements showed a rapid tuning of optical diffraction from these nanostructures from 41 to 48°. The nanostructures were patterned near the edges of the contact lens to avoid any interference and obstruction to the human vision. The formation of 2D nanostructures on lenses increased the diffraction efficiency by more than 10%. The versatility of the holographic laser ablation method was demonstrated by producing four different 2D nanopattern geometries on contact lenses. Hydrophobicity of the contact lens was characterized by contact angle measurements, which increased from 59.0° at pristine condition to 62.5° at post-nanofabrication. The holographic nanostructures on the contact lens were used to sense the concentration of Na+ ions. Artificial tear solution was used to simulate the conditions in dry eye syndrome, and nanostructures on the contact lenses were used to detect the electrolyte concentration changes (±47 mmol L–1). Nanopatterns on a contact lens may be used to sense other ocular diseases in early stages at point-of-care settings.