As major carbon (C) pools in cities, urban green spaces play a crucial role in reducing atmospheric carbon. To determine the importance of litterfall C storage in urban green spaces, we selected the leaf area index (LAI) as a proxy indicator for litterfall C density (LCD), and established a log-linear regression model between LCD and LAI to predict the annual litterfall C pool in large-scale urban green spaces using Sentinel-2 satellite remote sensing data. Forty-five sample units were randomly selected in typical urban green spaces in Beijing, China. A high-temperature combustion method was used to measure the LCD of the sampling units, and stepwise linear regression was used to filter the proxy indicator for LCD. The annual litterfall C pool in regions within the Fifth Ring Road was also estimated with inversion using remote sensing data. From 2015 to 2021, the estimated annual litterfall C pool was in the range of 4.5–5.8 × 1010 g, i.e., approximately 18.9% of the total C storage recorded for the urban green space, which was far greater than that observed in forest ecosystems. We concluded that the litterfall C pool in urban green spaces is seriously underestimated, and that urban tree litterfall has the potential to reduce greenhouse gas emissions if used as a carbon-neutral resource.