In this study, a novel surface modified and partly reduced graphene oxide (PRGO) induced by mild oligomeric proanthocyanidins (OPC) was prepared for efficient dye removal. The in situ partial reduction, modification and assembly of GO sheets into OPC-PRGO aerogels were readily realized by a hydrothermal process. Systemically characterizations were performed to confirm the partial reduction and modification of GO by OPC. The OPC-PRGO aerogels exhibited a honeycomb-like structure rather than a snowflake-like structure of GO aerogel. Due to its unique structure, the OPC-PRGO aerogels exhibited an excellent adsorption property towards organic dyes, such as methylene blue (MB), neutral red (NR), amino black (AB) and Congo red (CR). The removal efficiencies of OPC-PRGO towards MB, NR, AB and CR were observed to be 97.5, 94.5, 87.2 and 88.2%, respectively. This study opens a new insight for understanding and preparing partly reduced GO instead of completely reduced GO for hydrophilic polymer/graphene composites.