Promoting urban green growth necessitates a dual focus on reducing carbon emissions and fostering high-quality development. However, the body of research on the coupling relationship between high-quality urban development and carbon emissions remains remarkably limited. Taking Guangdong province as an example, this study strived to establish a comprehensive evaluation system for high-quality urban development encompassing economic, societal, and ecological dimensions and further conducted an in-depth examination of the spatiotemporal pattern and driving forces of coupling coordination degree between high-quality urban development and carbon emission intensity during 2000–2017. The coupling coordination degree in Guangdong province has shown continuous growth, transitioning from moderate incoordination to moderate coordination. The coupling coordination degree showed the overall spatial distribution characteristics of “high in southeast and low in others”, with Zhuhai, Zhongshan, Foshan, Guangzhou, Dongguan, and Shenzhen as the core. Notably, technological advancement, environmental governance, and economic development emerge as pivotal factors that positively affect carbon emission intensity reduction, environmental quality improvement, and coupling coordination enhancement. This research provides valuable insights for achieving harmonized high-quality development in Guangdong province involving policies of regional differences, industrial competitiveness, and new-type urbanization.