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Carbon dioxide (CO2) emissions to the atmosphere are causing increased public concern due to the consequence of global climate change, and solid adsorbents are one of the most promising options for CO2 capture. A fresh method for the fabrication of amine-modified CO2 solid adsorbents was proposed. Graphene oxide (GO) was modified by different concentrations of polyethylenimine (PEI) by a one-step method. The physical chemical structure and adsorption/desorption properties were characterized in detail. Results showed that the PEI-GO solid adsorbents were successfully fabricated and the particles were uniform, controllable and intact. The CO2 adsorption properties of PEI-GO solid adsorbents were measured, and the solid adsorbents exhibited good CO2 adsorption capacity (128.1mg/g) at 75 degrees C. In addition, the PEI-GO solid adsorbents were regenerable and exhibited good stability. Accordingly, this work stands out as a promising solution to a distinct way for the fabrication technology of CO2 solid adsorbents.