Rapid urbanization and associated greenhouse gas emissions pose severe challenges to global climate goals. Accurately estimating urban carbon emissions at fine administrative scales is a critical prerequisite for spatially differentiated mitigation policies and achieving carbon neutrality. However, while current research has validated the feasibility of using nighttime light (NTL) remote sensing for carbon estimation, most studies predominantly focus on macro scales, paying limited attention to intra-urban spatial heterogeneity and the value of high-resolution imagery. Using Nanjing, China, as a case study, this study examines the optimal scale, model, and data source for estimating urban total carbon emissions. NTL features from NPP/VIIRS and Luojia1-01 imagery were extracted at the district and township levels. Spatial lag and spatial error models were compared, and geographically weighted regression was further applied at the township level. The results show that urban carbon emissions in Nanjing exhibit clear scale effects and spatial non-stationarity. At the township level, the total indicator (TCE-TNLI) better reflects emission expansion in peripheral areas, while the intensity indicator (CI-ANLI) shows better predictive performance and robustness. With high-resolution Luojia1-01 imagery, the intensity model further reduces the effects of pixel saturation and administrative scale differences, achieving better model performance. These findings establish a robust methodological framework for fine-scale urban carbon accounting, demonstrating that integrating high-resolution imagery with intensity-based models is crucial for supporting spatially differentiated low-carbon planning in high-density megacities.