Moderate Resolution Imaging Spectroradiometer (MODIS) products and climate data collected from meteorological stations were used to characterize the spatial–temporal dynamics of gross primary productivity (GPP), evapotranspiration (ET), and water-use efficiency (WUE) in the Yangtze River Delta (YRD) region and the response of these three variables to meteorological factors. The seasonal patterns of GPP and WUE showed a bimodal distribution, with their peak values occurring in May and August, and April and October, respectively. By contrast, the seasonal variation of ET presented a unimodal pattern with its maximum in July or August. The spatial distribution of ET and GPP was similar to higher values occurring in the south. From 2001 to 2012, GPP in the eastern YRD decreased, while GPP in the western part increased. In comparison, over the 12 years, ET in the northern part of YRD decreased, while ET in the southern part increased. The spatial distribution and spatial variation of WUE were both similar to those of GPP. This implies that the changes in WUE are primarily controlled by the variations in GPP. The annual average WUE over vegetation types followed the order of: evergreen broadleaf forest (1.95 g C kg−1 H2O) > deciduous broadleaf forest (1.87 g C kg−1 H2O) > evergreen needle leaf forest (1.70 g C kg−1 H2O) > deciduous needle leaf forest (1.68 g C kg−1 H2O) > grassland (1.66 g C kg−1 H2O) > cropland (1.61 g C kg−1 H2O). Both GPP and ET increased with increasing annual mean temperature (Ta) and annual mean precipitation across all of the plant function types. WUE decreased as vapour pressure deficit (VPD) increased in all of the biomes. Interestingly, the relationship between WUE and VPD was the most significant in broadleaf forest. Whether this phenomenon is universal should be investigated in future studies.