Leaf chlorophyll content (LCC) is a prominent plant physiological trait and a proxy for leaf photosynthetic capacity. The acquisition of LCC data over large spatial and temporal scales facilitates vegetation growth monitoring and terrestrial carbon cycle modeling. In this study, a global 500 m LCC weekly dataset (GLCC) was produced from ENVISAT MERIS and Sentinel-3 OLCI satellite data using a physical radiative transfer modeling approach that considers the influence of canopy structure and soil background. Firstly, five look-up-tables (LUTs) were generated using PROSPECT-D+4-Scale and PROSAIL-D models for woody and non-woody plants. For the four LUTs applicable to woody plants, each LUT contains three sub-LUTs corresponding to three types of crown height. The one LUT applicable to non-woody vegetation type includes 25 sub-LUTs corresponding to five kinds of canopy structures and five kinds of soil backgrounds. The final retrieval was considered the aggregation of the LCC inversion results of all sub-LUTs for each plant function type (PFT). Then, the GLCC dataset was generated and validated using field measurements, yielding an overall accuracy of R2 = 0.41 and RMSE = 8.94 μg cm−2. Finally, the GLCC dataset presented acceptable consistency with the existing MERIS LCC dataset. OLCI, as the successor to MERIS data, was used for the first time to co-produce LCC data from 2003–2012 to 2018–2020 in conjunction with MERIS data. This new GLCC dataset spanning nearly 20 years will provide a valuable opportunity to analyze variations in vegetation dynamics.