By using a hierarchical equations-of-motion approach, we reproduce the two-dimensional electronic spectra of phycoerythrin 545 from Rhodomonas CS24 at ambient temperature (294 K). The simulated spectra are in agreement with the experimental results reported in Wong et al. (Nat. Chem. 2012, 4, 396). The evolutions of cross peaks for rephasing spectra and diagonal peaks for nonrephasing spectra have also been plotted. The peaks oscillate with the population times, with frequencies, phases, and amplitudes of the oscillating curves also being qualitatively consistent with the experimental results.