Rapid urbanization, land scarcity, and accompanying ecological deterioration in China have received growing attention. In this paper, two fast-growing metropolitan regions, Greater Shanghai and Greater Hangzhou, were selected as case studies to quantify the impact of land use/land cover (LULC) change on regional ecosystem services value (ESV) at the landscape scale since the late 1970s. The results show that in both regions, dramatic LULC change, especially recent land development at the urban fringes, led to a steady decline in the available area of productive agricultural land, natural land and semi-natural land. This consequently caused remarkable landscape fragmentation along the urban-rural gradient as measured by five class-level landscape metrics. It was estimated that in Greater Shanghai, regulating, supporting, provisioning, and cultural ESVs decreased by 32.05%, 17.89%, 53.72%, and 17.06%, respectively. In Greater Hangzhou, these values decreased by 27.82%, 23.86%, 28.62%, and 22.85%, respectively. In addition, the relationship is quantified between zonal buffer-based ESV and class-level landscape metrics. Further analysis shows that spatiotemporal patterns of zonal ESVs along the urban-rural gradient in these two regions exhibited unbalanced patterns of ecological services delivery.