Research on land use carbon emission efficiency (LUCEE) in the Pan-Pearl River Delta (PPRD) can aid in formulating regional differentiated carbon reduction strategies. In this work, the inversion of carbon emissions using night-time light (NTL) data and the modified Carnegie Ames Stanford Approach (CASA) model were used to measure the net carbon emissions from land use (NCELU). On this basis, the SBM-undesirable model was used to assess the LUCEE. Additionally, the exploratory spatial data analysis (ESDA), Dagum Gini coefficient, and spatial convergence model were further introduced to analyze the spatial correlation, regional differences, and convergence trend of the LUCEE. Findings indicate that: (1) The NCELU showed an increasing fluctuation. During the period of 2006–2020, the NCELU increased from −168.58 million tons to −724.65 million tons. (2) The LUCEE exhibited a three-phase fluctuating downward trend of “decrease–rise–decrease”. The LUCEE first decreased from 0.612 in 2006 to 0.544 in 2008, then gradually increased to 0.632 in 2016, and finally decreased to 0.488 in 2020. Spatially, the LUCEE manifested a distribution characteristic of “high in the north and south, low in the middle”, with distinct spatial clustering features. (3) The overall Gini coefficient in the study period increased from 0.1819 to 0.2461. The primary contributor to the overall difference over the entire sample period was hypervariable density. (4) The PPRD and its various subregions displayed significant features of absolute and conditional β convergence. The speed of regional convergence from fastest to slowest was central > west > east, with the absolute convergence speeds of 0.0505, 0.0360, and 0.0212, respectively. Finally, policy recommendations are proposed to achieve regional carbon neutrality for the PPRD.