[1] Ocean acidification resulting from increases in present and future atmospheric CO 2 levels could seriously affect diverse coastal and oceanic ecosystems. In this work, we determine that a significant trend in ocean acidification is superposed on the large seasonal and interannual variabilities of acidity in surface waters off the south coast of Honshu, Japan, based on our repeated observations of partial pressure of CO 2 ( pCO 2 ), total inorganic carbon (TCO 2 ), and pH. Multiple regression analysis of TCO 2 as a function of temperature, salinity, and timing of observations shows that TCO 2 increased at a rate of +1.23 ± 0.40 mmol kg −1 yr −1 for the period 1994-2008, while no long-term change has been determined for total alkalinity calculated from TCO 2 and pCO 2 in seawater. These results indicate that pH and the aragonite saturation state (W arag ) are decreasing at a rate of −0.020 ± 0.007 decade −1 and −0.12 ± 0.05 decade −1 , respectively. If future atmospheric CO 2 levels keep increasing as predicted by the Intergovernmental Panel on Climate Change emission scenario A1FI, which postulates intensive fossil fuel use associated with very rapid economic growth, a further reduction of −0.8 to −1.0 in W arag is likely in the next 50 years. Such a rapid reduction of W arag could have negative impacts on a variety of calcareous organisms.