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The ability of treeline conifers in the Central European Alps to cope with recent climate warming and increasing CO2 concentration is still poorly understood. We determined basal area increment (BAI) and tree ring stable carbon isotope ratios (δ13C) of Pinus cembra trees from 1925 through 2013. Stable isotope ratios and BAI were compared with leaf level gas exchange measurements carried out in situ between 1934 and 2012, and thus, provided new insights into long-term trends of tree-ring derived intrinsic water-use efficiency (iWUE). Mature P. cembra trees at treeline responded to increasing Ca and air temperature with a parallel increase in maximum net CO2 uptake rate at ambient CO2 (Amax) and tree-ring-derived intercellular CO2 partial pressure (Ci). Amax tripled and was positively correlated to BAI and Ci. The latter increased in parallel with ambient CO2 concentration and stomatal conductance. In contrast to the instantaneous gas exchange parameters, δ13C derived iWUE informs about the long-term changes in the carbon water relations. These data showed three changes in the iWUE chronosequences, which could be identified with different long term gas exchange patterns: (1) from stomatal controlled functioning from 1925 to 1981, to a situation where (2) both net CO2 fixation (A) and leaf conductance for water vapour (gw), responded to the environment from 1982 to 1997, and (3) back to a stomata controlled pattern over iWUE from 1998 onwards. This temporal pattern was also mirrored in leaf level gas exchange assessments, suggesting a parallel increase of A and gw of P. cembra at treeline during the last nine decades.