This work presents the results of the study of plasterwork decorations located on the stalactite vaults of the Hall of the Kings in the Alhambra (Granada, Spain) by means of Raman micro-spectroscopy. Field investigations were carried out in situ using a portable Raman spectrometer during a conservation campaign in a completely non-invasive manner. In addition, taking into account the results obtained, a well-directed sampling was carried out to obtain complementary information by means of laboratory studies. Despite several practical problems during the non-invasive field studies (like difficulties for probe positioning and vibrations of the scaffolding), almost all the pigments present in the decorations of the Hall were identified using excitation at 785 nm: cinnabar, minium, carbon black, natural lapis lazuli and synthetic ultramarine blue. In addition, evidence of different degradation mechanisms of the red pigments was obtained in situ. On the contrary, the identification of blue-greenish and green pigments had to be performed on microsamples using a Raman microscope with excitation at 514 nm in the laboratory. In samples with blue and green areas, azurite severely degraded to clinoatacamite was identified. These were probably the remains of the oldest blue decorations. In addition, a technique for green decorations consisting on copper chlorides mixed with a small amount of lapis lazuli was identified. Other degradation products, identified in the laboratory regardless of the color of the pigment, were calcium oxalates. Finally, the laboratory studies also enabled the investigation of the stratigraphy of the pictorial layers. In this way, the presence of re-decorations with overlaying layers of pigments even of different colors was revealed. Copyright © 2014 John Wiley & Sons, Ltd.