This data set represents a simultaneously taken data set for overlying air, sea surface microlayer (SML, < 1 mm depth), and underlying water (ULW, 1 m depth) for microplastic (MP) including tire wear particles (TWP). Samples were taken in three different Swedish fjords of varying anthropogenic impact (urban (UB), industrial (AF), and rural (GF)) with a remote-controlled research catamaran (Sea Surface Scanner (S³), doi:10.1175/JTECH-D-17-0017.1). Each day, one air sample was taken by actively sampling air during the entire daily GPS track of the S³. For the water samples, every day three SML (3x10 L) and three ULW (3x10 L) samples were taken, while the S³ was driving along the respective GPS tracks and pooled together for each day. GPS tracks are available for each day, except day 5. Here, weather conditions did not allow a deployment of the S³ and it was operated while being tied to the quay. The analysis was conducted with pyrolysis-gas chromatography-mass spectrometry (Py-GC/MS). Details concerning the measurements, quantification, and calibration are found in the related study (Goßmann et al., 2023; doi:10.1021/acs.est.3c05002). The indicator used for identification and quantification of the polyvinyl chloride cluster (C-PVC) is rather unspecific. Therefore, C-PVC might be interfered by additional anthropogenic sources and the given C-PVC concentration only represents an order of magnitude. Enrichment factors (EF) of MP and TWP were calculated by dividing the concentration in the SML by the concentration of the ULW. EF above one describe an enrichment in the SML, EF below one indicate a depletion.