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In this work, we focus our attention on pyrrole (C4H5N)—an important aromatic compound, because it is a fundamental constituent of petroleum.Up to now, there appear to rare researches on pyrrole under high-pressure.At ambient conditions, pyrrole exists in liquid form.At 103 K, pyrrole crystallizes into phase N with space group Pnma.In this paper, we present the first direct observations of pyrrole by means of in situ high-pressure synchrotron XRD and Raman scattering spectra up to ～34 GPa.