Herein, we present the acquisition of ultrafast nonlinear vibrational action spectroscopy on cryogenically cooled, dilute molecular ion ensembles. Using a pulse shaper to control the ultrafast pulse sequence and isolate the desired nonlinear signal, we observe relatively strong bleaching signals in the C≡O stretch region of the metal-carbonyl complex fac-Re(CO)3(CH3CN)3 + tagged with a single N2 molecule. Importantly, the carbonyl bleaching signals oscillate with pump-probe waiting time with a period corresponding to the energy difference between the excited vibrational features, consistent with coherent coupling between the vibrational modes. With this successful demonstration, we provide the framework needed to collect multidimensional IR spectra and transient UV/Vis-IR spectra of charged molecular systems.