Mean phase-averaged horizontal airflow velocities and power spectral densities (PSD) of high-pass filtered (with respect to frequency) wave slope measurements, obtained from laboratory experiments in University of Hamburg's (Germany) wind-wave tank. A total of 20 wind-wave conditions were examined with varying wind speeds and three different surfactants deployed on the water surface. Experiments 1–5 were performed on a slick-free surface (no surfactant), experiments 6–10 with oleyl alcohol (OLA), experiments 11–15 with palmitic acid methyl ester (PME), and experiments 16–20 with toluol (TOLG).The horizontal airflow velocity component (aligned with the mean wind direction) was measured at various heights above the water surface, using a 2D FlowExplorer Laser Doppler Velocimetry (LDV) system (Dantec Dynamics). Raw velocity data were binned with respect to wave phase, and averaged to generate mean along-wave airflow velocity maps. Wave slope data, recorded with a laser slope gauge, were divided into short segments (chunks), each matching exactly the wave-phase interval of a specific phase bin. Chunks from multiple wave cycles that corresponded to the same phase bin were grouped together. For each bin separately, these grouped chunks were concatenated into continuous sequences. Spectral analysis was then performed on each concatenated sequence to compute the power spectral density (PSD) of the high-pass filtered (f > 10 Hz) wave slope.This dataset includes variables with their respective coordinates: height above the waves and wave phase for the airflow velocity maps; frequency and wave phase for the PSDs. Additionally, the wave-following coordinate and the phase-averaged surface elevation are provided. For each experimental run, friction velocity and horizontal airflow velocity extrapolated to a reference height of 10 m are provided.