The lack of observational pH data has made it difficult to assess recent rates of ocean acidification, particularly in the high latitudes. Here we present a time series that spans over 27 yr (1981-2008) of high-quality carbon system measurements in the North Atlantic, which comprises fourteen cruises and covers the important water mass formation areas of the Irminger and Iceland Basins. We provide direct quantification of acidification rates in upper and intermediate North Atlantic waters. The highest rates were associated with surface waters and with Labrador Sea Water (LSW). The Subarctic Intermediate and Subpolar Mode Waters (SAIW and SPMW) showed acidification rates of -0.0019 +/- 0.0001 and -0.0012 +/- 0.0002 yr(-1), respectively. The deep convection activity in the North Atlantic Subpolar Gyre injects surface waters loaded with anthropogenic CO2 into lower layers, provoking the remarkable acidification rate observed for LSW in the Iceland Basin (-0.0016 +/- 0.0002 yr(-1)). An extrapolation of the observed linear acidification trends suggests that the pH of LSW could drop 0.45 units with respect to pre-industrial levels by the time atmospheric CO2 concentrations reach similar to 775 ppm. Under circulation conditions and evolution of CO2 emission rates similar to those of the last three decades, by the time atmospheric CO2 reaches 550 ppm, an aragonite undersaturation state could be reached in the cLSW of the Iceland Basin, earlier than surface SPMW.