Gas-phase N-2 adsorption on protonated tryptophan and dipeptides, hydrogen-bonded with methanol, was investigated as a model for molecular cloud formation using a tandem mass spectrometer containing a cold ion trap. The number of N-2 molecules adsorbed on H+ Trp(CH3OH)(m) and H(+)Trp-Gly(CH3OH)(m)(m = 0-3) decreased with increasing number of methanol molecules. The surface of the gas-phase ions was covered by the CH3 groups of methanol upon solvation, which rendered the solvated cluster ions inactive toward N-2 adsorption. The lack of N-2 adsorption on unsolvated H(+)Gly-Trp was ascribed to its compact conformation, which was driven by the intramolecular interactions.