A suite of large-eddy simulation(LESs) of decaying homogeneous isotropic turbulence at high Reynolds numbers is performed and compared to wind-tunnel experiments in the tradition of Comte-Bellot and Corrsin. The error-landscape approach is used for the evaluation of the Smagorinsky model, and the results are used to identify an optimal combination of model parameter and resolution in a statistically robust fashion. The use of experimental reference data in the error-landscape approach allows to evaluate the optimal Smagorinsky coefficient at high Reynolds numbers and to perform detailed comparisons with analytical predictions. We demonstrate, using a pseudospectral discretization, that the optimal so-called Smagorinsky trajectory obtained f...