It is possible to take advantage of shallow reservoirs (<300 m) for CO2 capture and storage in the post-combustion process. This process is called enhanced carbon capture and storage (e-CCS). In this process, it is necessary to use a nano-modifying agent to improve the chemical-physical properties of geological media, which allows the performance of CO2 selective adsorption to be enhanced. Therefore, this study presents the development and evaluation of carbon sphere molecular nano-sieves (CSMNS) from cane molasses for e-CSS. This is the first report in the scientific literature on CSMNS, due to their size and structure. In this study, sandstone was used as geological media, and was functionalized using a nanofluid, which was composed of CNMNS dispersed in deionized water. Finally, CO2 or N2 streams were used for evaluating the adsorption process at different conditions of pressure and temperature. As the main result, the nanomaterial allowed a natural selectivity towards CO2, and the sandstone enhanced the adsorption capacity by an incremental factor of 730 at reservoir conditions (50 °C and 2.5 MPa) using a nanoparticle mass fraction of 20%. These nanofluids applied to a new concept of carbon capture and storage for shallow reservoirs present a novel landscape for the control of industrial CO2 emissions.