AMBER14SB (35%) understabilizes the native state, and AMBER99 grossly overstabilizes the misfolded state with no appreciable folded state population. None of the CHARMM force fields we tested predict appreciable misfolded state populations: CHARMM22* (77%) and CHARMM27 (84%) predict an overstabilized native state, while CHARMM36 predicts a mostly unfolded-state ensemble (7% folded, 93% unfolded). While reduced chi-squared values for the NOE distances show similar trends to those in Figure , the reduced chi-squared values are larger overall for the proton chemical shifts (H α and H N ) and J-coupling constants. CHARMM27 outperforms the other force fields in reproducing experimental chemical shifts, with χ 2 /N ∼ 4 for H α and χ 2 /N ∼ 3 for H N . OPLS-aa and AMBER99SB-nmr1-ildn outperform the other force fields in reproducing J-coupling constants, although all reduced chi-squared values are large (χ 2 /N > 6 in all cases), and show greater variability across MSMs constructed with different numbers microstates. The poorest agreement with J-coupling constants is for AMBER99 and CHARMM36 (χ 2 /N ∼ 28), both of which do not predict appreciable native state populations.