In this study, we report a facile and efficient method using supercritical (SC) CO2 to help a p-type conducting polymer, conjugated polymer MDMO-PPV wrapping on carbon nanotubes (CNTs). One-dimensional CNTs were periodically decorated with the congeries of MDMO-PPV molecular chains forming functional nanohybrid structures. The solubility and light emission of the hybrid MDMO-PPV/CNTs can be controlled by varying SC CO2 pressure. Using FT-IR, we can observe there exists chemical interaction between MDMO-PPV and CNTs, and the interaction not only bestowed CNTs desired solubility but also added functionality of light emission to CNTs. The fluorescence spectroscopy of the MDMO-PPV/CNTs shows their light emission is strongly depend on solvent. For DMSO as the solvent, the higher SC CO2 pressure ensures the excellent dispersion and solubility of MDMO-PPV/CNTs, and accordingly causes the light quenching of the hybrid. For DMAc as the solvent, the enhanced emission light can be observed from the MDMO-PPV/CNTs, especially at higher SC CO2 pressure. We anticipate this work opens a gateway for making use of SC CO2 to help functionalize CNTs with conjugated polymer for use in polymer solar cells, light-emitting diodes, and others.