Measurements of spectral zenith radiance in the 320–950 nm wavelength range have been carried out since 2021 at the Thule High Arctic Atmospheric Observatory (THAAO, https://www.thuleatmos-it.it/, 76.5° N, 68.8° W, 225 m a.s.l) located in Pituffik, northern Greenland. This study evaluates whether such observations could provide, in principle, scientifically meaningful cloud optical depth (τ) estimates, what would be the limitations, which are the necessary auxiliary measurements, and which radiance wavelengths would be better suited for the goal. Although clouds play a critical role in the Arctic, a climatology of τ in high albedo conditions is particularly difficult to obtain. THAAO might have the instrument capabilities to provide such a long-term dataset. We use a radiative transfer package to simulate visible spectra with different cloud and surface conditions, assuming homogeneous overcast sky and liquid water clouds of fixed geometrical thickness. Simulations are run to reproduce typical conditions encountered at THAAO when measurements are carried out. We find that the assumption of a broadband albedo instead of a spectrally-resolved one is the source of the largest uncertainties. Tests on size and phase of cloud particles showed that a 50% uncertainty in reff leads to a ∼10% error in τ, and that a 10% contamination of ice crystals in a low-level liquid water cloud leads to an error in τ estimates of less than 5%. All the tests showed that the most critical τ range is between the thin and thick cloud regimes (τ ∼ 7–15), where the retrievals can be less reliable. Otherwise, tests suggest that in the environmental conditions that characterize late spring and summer at THAAO, and given the observatory measurements capabilities, estimates of τ for low-level clouds could be accurately retrieved both in high and low surface albedo conditions by means of zenith radiance measurements in the UV-Vis-NIR range.