To address critical limitations of ultra-low viscosity supercritical CO₂ fracturing fluids, including excessive fluid loss and inadequate proppant transport capacity, a series of thickeners designed to significantly enhance CO₂ viscosity were synthesized. Initially, FT-IR and ¹H NMR characterization confirmed successful chemical reactions and incorporation of both solvation-enhancing and -thickening functional groups. Subsequently, dissolution and thickening performance were evaluated using a custom-designed high-pressure vessel featuring visual observation capability, in-line viscosity monitoring, and high-temperature operation. All thickener systems exhibited excellent solubility, with 5 wt% loading elevating CO₂ viscosity to 3.68 mPa·s. Ultimately, molecular simulations performed in Materials Studio elucidated the mechanistic basis, electrostatic potential (ESP) mapping, cohesive energy density analysis, intermolecular interaction energy, and radial distribution function comparisons. These computational approaches revealed dissolution and thickening mechanisms of polymeric thickeners in CO₂.