archetypical" hybrid 3D perovskites, a vivid interest has emerged for their derivatives with reduced dimensionality.The general formula of 2D perovskites is A 2 BX 4 , where A is a monovalent organic cation, B is a divalent metallic cation (for example Pb), and X is a halide anion (Cl, Br, or I). 2D perovskites consist of alternating organic (A) and inorganic layers ([BX 6 ] 4octahedra), where A acts as an electronically insulating spacer that strongly confine excitons in the inorganic part, forming a natural multiple quantum well.In particular, layered 2D Ruddlesden-Popper perovskites combine some of the outstanding physical properties of hybrid 3D perovskites with the unique tunability of low-dimensional materials. [3][4][5] As a result of dielectric confinement, the excitons in 2D perovskites are stable and show strong photoluminescence up to room temperature, unlike the artificially constructed quantum well structures of the classical III−V semiconductors (for example, the GaAs-based heterostructures). For these reasons 2D perovskites have become one of the forefronts Combining the characteristics of hybrid perovskites and layered materials, 2D Ruddlesden-Popper perovskites exhibit unique properties, some of which still require to be deeply understood. In this study, the vibrational signatures of such materials are analyzed by collecting experimental Raman spectra of four distinct compounds. Supported by density functional theory simulations, the role of the phenyl spacer single fluorination on the phonon modes of two similar yet different compounds, i.e., phenethylammonium lead iodide (PEAI) and 4-fluorophenethylammonium lead iodide (PEAI-F), is explained. In addition, this work analyzes some so-far unreported experimental Raman peaks in the 600-1100 cm −1 range and discusses their origin in this class of 2D compounds. This work paves the way for a better design of novel compounds as well as for their exploitation in (opto)electronic applications.