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Rapid urbanization has threatened sustainable urban development in many cities across the globe, causing green space loss and vegetation cover degradation which reduce carbon sequestration. Optimal land management practices (LMPs) in an urban context are known as ways capable of promoting urban vegetation growth and contributing to carbon sequestration. Due to variations of physical, biological, and social structures in urban areas, policymakers often lack relevant information to decide and implement site-specific LMPs. Here we try to extract the areas in need of the optimal LMPs, identify location-dependent optimal LMPs, and assess how much more carbon can be captured by applying a combination of segmenting homogeneous urban environments and neighborhood-based analysis. As one of the most developed cities in China, the greater Guangzhou area (GGA) was selected as a case study. We found that the carbon uptake from the urban vegetation in GGA could be improved on average by 185 gC m−2 yr−1 in flux (or 1.3 TgC yr−1 in total) with optimal LMPs, equivalent to a ~30% increase considering the current level of 662 gC m−2 yr−1 in flux (4.4 TgC yr−1 in total). The carbon uptake potential was found to differ considerably across locations and among different ecosystem types, highlighting spatially varied priorities for implementing optimal LMPs over the space. This study reveals the usefulness of the model in assessing carbon uptake potential from optimal LMPs and emphasizes that future urban planning may consider the importance of optimal LMPs in enhancing vegetation carbon uptake in urban planning. [ABSTRACT FROM AUTHOR]