Urbanization has significantly altered urban landscape patterns, leading to a continuous reduction in the proportion of green spaces. As critical carbon sinks in urban carbon cycles, urban green spaces play an indispensable role in mitigating climate change. This study aims to evaluate the carbon capture and storage potential of urban green spaces in Luohe, China, and identify the landscape factors influencing carbon sequestration. The research combines on-site data collection with high-resolution remote sensing, utilizing the i-Tree Eco model to estimate carbon sequestration rates across areas with varying levels of greenery. The study reveals that the carbon sequestration capacity of urban green spaces in Luohe City is 1.30 t·C·ha−1·yr−1. Among various vegetation indices, the Enhanced Vegetation Index (EVI) explains urban green space carbon sequestration most effectively through an exponential model (R2 = 0.65, AIC = 136.5). At the city-wide scale, areas with higher greening rates, better connectivity, and more complex edge morphology exhibit superior carbon sequestration efficiency. The explanatory power of key landscape indices on carbon sequestration is 78% across the study area, with variations of 71.5%, 62%, and 84.9% for low, medium, and high greening rate areas, respectively. Moreover, when greening rates reach a certain threshold, maintaining and optimizing the quality of existing green spaces becomes more critical than simply expanding the green area. These insights provide valuable guidance for urban planners and policymakers on enhancing the ecological functions of urban green spaces during urban development.