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We have developed a modulation phase-shift (MPS) system for measuring relative group delay (RGD) in optical components with high absolute accuracy and simultaneously high temporal and wavelength resolution. Our 200-MHz system has a 3.2-pm wavelength resolution and has demonstrated a group-delay resolution of 0.072 ps for repeated measurements of an artifact based on a hydrogen-cyanide gas cell. The expanded uncertainty (2σ) is ±0.46 ps for a single spectral measurement (∼ 3.4-pm steps) of a narrow 20-ps group-delay feature of the artifact. To our knowledge, this is the first time that the sources of measurement uncertainty for this technique have been described and quantified. A method for predicting the group delay of the gas-cell artifact from measured absorption spectra is described, and an uncertainty analysis for the prediction method is also presented. The implementation required to achieve results of the highest accuracy for both measurements and predictions is discussed.