Hayes et al . (Reports, 21 June 2013, p. 1431) used two-dimensional (2D) electronic spectroscopy to study molecular heterodimers and reported a general mechanism for the prolongation of electronic coherences, consistent with previous interpretations of 2D spectra for light-harvesting systems. We argue that the dynamics attributed to electronic coherences are inconclusive based on experimental inconsistencies arising from limited sample characterization and insufficient control measurements.