Widespread drought-induced tree mortality has been documented around the world, and could increase in frequency and intensity under warmer and drier conditions. Ecophysiological differences between dying and surviving trees might underlie predispositions to mortality, but are poorly documented. Here we report a study of Scots pines (Pinus sylvestris L.) from two sites located in north-eastern Iberian Peninsula where drought-assocated mortality episodes were registered during the last few decades. Time trends of discrimination against 13C (D13C) and intrinsic water-use efficiency (WUEi) in tree rings at an annual resolution and for a 34 year period were used to compare co-occurring now-dead and surviving pines. Results indicate that both surviving and now-dead pines significantly increased their WUEi over time, although this increase was significantly lower for now-dead individuals. These differential WUEi trends corresponded to different scenarios describing how plant gas exchange responds to increasing atmospheric CO2 (Ca): the estimated intercellular CO2 concentration was nearly constant in surviving pines but tended to increase proportionally to Ca in now-dead trees. Concurrently, the WUEi increase was not paralleled by a growth enhancement, regardless of tree state, suggesting that in water-limited areas like the Mediterranean, it cannot overcome the impact of an increasingly warmer and drier climate on tree growth.