Exploring the spatial interaction between Ecosystem Services (ESs) and urbanisation can provide a new perspective for urban development and protection. Taking the Changsha-Zhuzhou-Xiangtan (CZT) urban agglomeration as a case study, with reference to its land use and social economy in 2015, this paper employs grid analysis and a spatial autocorrelation model to analyse the spatial relationships between urbanisation and ESs. The results show that:(1) The spatial distribution of the levels of urbanisation are characterised by evident regional differences within the CZT urban agglomeration, with the level of urbanisation decreasing from urbanised areas to urbanising areas and to ecological conservation areas. (2) The spatial distribution pattern of ESs, influenced by the level of urbanisation and land use change, showed a obvious difference, with the values associated to ESs gradually increasing from the urban centres to the peripheries. (3) Urbanisation and individual ESs show significant negative correlation. Due to the different driving mechanisms, urbanisation in urbanised areas, urbanising areas, and ecological conservation areas had significicantly different impacts on the individual ESs. (4) Four spatial correlation types between individual ESs and urbanisation levels in the CZT urban agglomeration are identified. High-High areas and Low-Low areas are scattered throughout the study area, but cover only a small portion of it; High-Low areas are concentrated in the southwest of Xiangtan County and southeast of Zhuzhou County, and cover a larger proportion of the study area; Low-High areas are concentrated in the cities within the urban agglomeration, and as such they are widespread and cover large areas.