Cancer villages, or popularly called Aizheng Cun (癌症村) in Chinese, are a new phenomenon after the economic reform in China. This study aims to investigate the degree to which the changes in land use and land cover (LULC) degraded the water quality in cancer villages with a focus on Shenqiu County in Henan Province, one of the most notorious cancer villages in China. Changes in LULC and vegetative content on water surfaces and their spatial relationships were profiled using land surface remotely sensed data. The study finds that along with the considerable expansion of built environment and farmland over thirty years (1987–2017), the mean of the Normalized Difference Vegetation Index (NDVI) on water surfaces, a proxy for surface water biomass, increased dramatically (from −0.11 to 0.34). Moreover, around 80 percent of the newly fabricated built environment and 74 percent of the new farmland occurred in close proximity (within 1 km) to the water bodies with increased NDVI. Because vegetative content on water surfaces was used as a possible indicator for water quality degradation in water quality, the findings could support the assumption that wastewater discharges from anthropogenic activities contribute to the degrading water quality in cancer villages.