This dataset is part is the data supplement presented in Nguyen et al. 2021 (submitted to ESSD) in which we present 20-year flask sample records of atmospheric CO2, δO2/N2 and APO from the stations Lutjewad (the Netherlands) and Mace Head (Ireland) and a 3-year record from Halley station (Antarctica), including details of the extensive calibration procedure and its stability over time. The results of our inter-comparison involving gas cylinders from various research laboratories worldwide also show that our calibration is of high quality and compatible with the internationally-recognised Scripps scale. The measurement records from Lutjewad and Mace Head show similar long-term trends during the period 2002-2018 of 2.31 ± 0.07 ppm yr-1 for CO2 and -21.2 ± 0.8 per meg yr-1 for δO2/N2 at Lutjewad, and 2.22 ± 0.04 ppm yr-1 for CO2 and -21.3 ± 0.9 per meg yr-1 for δO2/N2 at Mace Head. They also show similar δO2/N2 seasonal cycle with an amplitude of 54 ± 4 per meg at Lutjewad and 61 ± 5 per meg at Mace Head, while CO2 seasonal amplitude at Lutjewad (16.8 ± 0.5 ppm) is slightly higher than that at Mace Head (14.8 ± 0.3 ppm). We show that the observed trends and seasonal cycles are compatible with the measurements from various stations, especially the measurements from Weybourne Atmospheric Observatory (United Kingdom). However, there are remarkable differences in the progression of annual trends between the Mace Head and Lutjewad records for δO2/N2 and APO, which might in part be caused by sampling differences, but also by environmental effects, such as the North Atlantic Ocean oxygen ventilation changes to which Mace Head is more sensitive. The Halley record shows clear trends and seasonality in δO2/N2 and APO, where especially APO agrees well with the continuous measurements at Halley by the University of East Anglia, while CO2 and δO2/N2 present slight disagreements, most likely caused by small leakages during sampling. From our 2002-2018 records, we find good agreement for the global ocean sink: 2.0 ± 0.8 PgC yr-1 and 2.2 ± 0.9 PgC yr-1, based on Lutjewad and Mace Head, respectively.