The vibrational spectra of the NH2-stretching modes of aniline–Ne and aniline–Ne+ have been measured using infrared depletion spectroscopy and REMPI–TOF mass spectrometry. In the NH2-stretching vibration region of the aniline–Ne clusters, two absorption bands at 3422 and 3508cm−1 were observed. The frequency shifts from the monomer was found to be negligibly small. As for the aniline–Ne+ cluster cations, the observed frequencies of the vibrational modes were 3394 and 3488cm−1. These values agreed with ones observed for aniline–Ar+ cluster within the error limit. This fact suggests that the effect of neon to aniline in forming the cluster is not significant in the vibrational spectra, and supports that we can use these values as the unperturbed NH2-stretching frequencies of the aniline monomer cation.