The datasets belong to a publication with the title "Characterization of molecular interactions in the bondline of composites from plasma-treated aluminum and wood". Wood and aluminum composites are becoming increasingly attractive due to their ability to combine the advantages of both materials: the lightweight nature of wood and the strength of aluminum. However, using conventional wood adhesives like polyvinyl acetate (PVAc) to bond these dissimilar materials is challenging and requires special surface treatments. This study focuses on the molecular interactions between PVAc and aluminum or spruce wood influenced by plasma surface modification. The surface sensitive methods X-ray photoelectron spectroscopy, infrared reflection adsorption spectroscopy and atomic force microscopy were employed to characterize the PVAc films on the corresponding surfaces and to identify possible interactions. The ultrathin PVAc films required for this purpose were deposited by spin coating on untreated and on plasma-treated aluminum.