The presented article reports the preparation and characterization of heterogeneous carbon catalyst enriched with carboxylic group denoted as (ECS) from Eucalyptus as an efficient catalyst for the hydrolysis of woody Eucalyptus biomass. The fabrication process is based on the ball milling of Eucalyptus as a carbon source in the presence of dry ice as an oxidizing agent followed by acidification with the assistance of hydrochloric acid. The data are including the schematic for the full synthesis steps and characterization tools in addition to the thermogravimetric analysis and proton nuclear magnetic resonance analysis for the ECS catalyst. Meanwhile, the catalytic performance of ECS catalyst towards the hydrolysis of Eucalyptus was measured under different temperatures ranged from 160 to 200 °C. The ECS catalyst allowed the selective hydrolysis of Eucalyptus to glucose and xylose, as proved by high-performance liquid chromatography. The data herein are associated with the article entitled " Unveiling one-pot fabrication of scalable and reusable carboxylated heterogeneous carbon-based catalyst from Eucalyptus plant with the assistance of dry Ice for selective hydrolysis of Eucalyptus Biomass'' [1].