AbstractAnalysis of microplastics (MP) in environmental samples is an emerging field, which is performed with various methods and instruments based either on spectroscopy or thermoanalytical methods. In general, both approaches result in two different types of data sets that are either mass or particle number related. Depending on detection limits of the respective method and instrumentation the derived polymer composition trends may vary. In this study, we compare the results of hyperspectral Fourier-transform infrared (FTIR) imaging analysis and pyrolysis gas chromatography-mass spectrometry (Py-GC/MS) analysis performed on a set of environmental samples that differ in complexity and degree of microplastic contamination. The measurements were conducted consecutively, and on exactly the same sample. First, the samples were investigated with FTIR using aluminum oxide filters; subsequently, these were crushed, transferred to glass fiber filters, in pyrolysis cups, and measured via Py-GC/MS. After a general data harmonization step, the trends in MP contamination were thoroughly investigated with regard to the respective sample set and the derived polymer compositions. While the overall trends in MP contamination were very similar, differences were observed in the polymer compositions. Furthermore, polymer masses were empirically calculated from FTIR data and compared with the Py-GC/MS results. Here, a most plausible shape-related overestimation of the calculated polymer masses was observed in samples with larger particles and increased particle numbers. Taking into account the different measurement principles of both methods, all results were examined and discussed, and future needs for harmonization of intermethodological results were identified and highlighted.