We present the adsorption characteristics of uranyl ions on a new and innovative composite which was composed of a carboxymethylated polyethyleneimine (CM-PEI) and an activated carbon (F400) with a nanopore less than 2 nm in diameter. In this study, we examined the adsorption phenomena of uranyl ions on the CM-PEI/F400 composite and evaluated the adsorption data using various isotherm models. It was found that the adsorption of uranyl ions on the CM-PEI/F400 composite obeys the Langmuir isotherm model. In addition, it was observed that pH of solutions had great influence on the adsorption capacity of uranyl ions on the CM-PEI/F400 composite. Specially, the adsorption capacity of uranyl ions was linearly increased with an increase of pH at pH > 3.0.