i-motif structures (IH and IC at pH 5.6) show monomodal CCSDs at low pH, but when the pH is increased and thus i-motifs are disrupted, the CCSDs become bimodal, with a higher-CCS contribution which increases with the charge state. A bimodal distribution can mean two things: the charge state can be produced both by a charged residue and a chain ejection mechanism, or the charge state is produced by the charged residue mechanism but is already in the middle of a collision-induced unfolding transition. However, the monomodal and low-CCS distribution for the folded i-motifs can only mean that they were produced exclusively by the charged residue mechanism. Thus, with 0.25% m-NBA, charge states up to 13-can be produced via the CRM, i.e., by native supercharging. However, if the structure is too unstable either in solution or in the gas phase (e.g., in CH, where the hairpin is quite short compared to the disordered region), this does not hold anymore. In summary the CCSD of charge states 9-to 13-show a memory of the solution structure already at low in-source activation voltages, with higher charge states showing a more clear-cut difference. For charge states 7-to 10-, collision-induced unfolding experiments better reveal the differences.