A high-quality inorganic carbon system database, spanning over three decades (1981–2006) and comprising of 13 cruises, has allowed the applying of the φC°T method and coming up with estimates of the anthropogenic CO2 (Cant) stored in the main water masses of the North Atlantic. In the studied region, strong convective processes convey surface properties, like Cant, into deeper ocean layers and grants this region an added oceanographic interest from the point of view of air-sea CO2 exchanges. Generally, a tendency for decreasing Cant storage rates towards the deep layers has been observed. In the Iberian Basin, the North Atlantic Deep Water has low Cant concentrations and negligible storage rates, while the North Atlantic Central Water in the upper layers shows the largest Cant values and the largest annual increase of its average concentration (1.13 ± 0.14 μmol kg−1 yr−1). This unmatched rate of change in the Cant concentration of the warm upper limb of the Meridional Overturning Circulation decreases towards the Irminger basin (0.68 ± 0.06 μmol kg−1 yr−1) due to the lowering of the buffering capacity. The mid and deep waters in the Irminger Sea show rather similar Cant concentration rates of increase (between 0.33 and 0.45 μmol kg−1 yr−1), whereas in the Iceland basin these layers seem to have been less affected by Cant. Overall, the Cant storage rates in the North Atlantic subpolar gyre during the first half of the 1990s, when a high North Atlantic Oscillation (NAO) phase was dominant, are ~48% higher than during the 1997–2006 low NAO phase that followed. This result suggests that a net decrease in the strength of the North Atlantic sink of atmospheric CO2 has taken place during the present decade. The changes in deep-water ventilation are the main driving processes causing this weakening of the North Atlantic CO2 sink.