AbstractOver the past few decades, the topic of recycling has become increasingly prominent in the field of sustainable materials and circular economy. One significant challenge is the physical separation of different types of plastics to obtain recyclates of one plastic type as pure as possible with comparable quality and properties to those of virgin material. Given the substantial effort involved in such separation, small amounts of contamination from other plastics may be tolerated. However, these contaminations must be monitored to ensure high-level recyclate quality. In recent years, compact, low-cost ion mobility spectrometers (IMS) with high analytical performance have been developed, and have thus become widely used in a variety of sensing applications. Due to their high sensitivity, IMS are particularly suited for detecting lowest concentration levels of various compounds, as required for the detection of impurities in recyclate quality monitoring. When coupled to a miniature gas chromatograph (GC), GC-IMS reach even higher separation power while being still compact. To bring recyclate samples to the gas phase, pyrolysis (Py) is used in this work. A first feasibility study was conducted to assess the potential of such a pyrolysis–gas chromatography-ion mobility spectrometer (Py-GC-IMS) with the objective of detecting contaminations of polyethylene terephthalate (PET) in polyethylene (PE) recyclates. The study clearly demonstrates the ability to identify PET-related fingerprints while suppressing the PE background matrix by design so that Py-GC-IMS seems a promising approach for in-process monitoring PET contaminations in PE recyclates.