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More than four decades of alkalinity and pH data (late 1960s to 2010) from coastal bays along the northwestern Gulf of Mexico were analyzed for temporal changes across a climatic gradient of decreasing rainfall and freshwater inflow, from northeast to southwest. The majority (16 out of 27) of these bays (including coastal waters) showed a long-term reduction in alkalinity at a rate of 3.0-21.6 μM yr(-1). Twenty-two bays exhibited pH decreases at a rate of 0.0014-0.0180 yr(-1). In contrast, a northernmost coastal bay exhibited increases in both alkalinity and pH. Overall, the two rates showed a significant positive correlation, indicating that most of these bays, especially those at lower latitudes, have been experiencing long-term acidification. The observed alkalinity decrease may be caused by reduced riverine alkalinity export, a result of precipitation decline under drought conditions, and freshwater diversion for human consumption, as well as calcification in these bays. A decrease in alkalinity inventory and accompanying acidification may have negative impacts on shellfish production in these waters. In addition, subsequent reduction in alkalinity export from these bays to the adjacent coastal ocean may also decrease the buffer capacity of the latter against future acidification.