Recent studies have demonstrated that microplastics (MPs) can act as a transport vector for pollutants in the environment. However, most studies have focused on carbon-carbon backbone polymers, with little known about heteroatom backbone polymers. In this study, polyurethane (PU) MPs were modified by UV irradiation and microorganism colonization to assess the different aging treatments on the interaction behavior (adsorption/desorption) between PU MPs and bisphenol A (BPA). The results of the adsorption kinetics experiment illustrated that the adsorption process of BPA could be described well by a pseudo-second order kinetic equation on both fresh and aged PU MPs. Although fresh PU MPs revealed the highest saturated adsorption capacity, at low BPA exposure concentrations (≤ 100 μg/L) the adsorption capacities for UV aged and biofilm colonized PU MPs were very similar to fresh MPs or even slightly higher than for fresh MPs, the main adsorption mechanisms including H-bonding interactions and π–π interactions. Fourier-transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM) investigations suggested obvious physicochemical property changes (e.g., generation of new functional groups, erosion, etc.) after UV irradiation and biofilm colonization. This study also showed that different exposure environments (ultrapure water, artificial seawater, simulated gastric fluid) could affect BPA adsorption/desorption via hydrophobic and electrostatic interaction on PU surfaces. These results further clarify the adsorption mechanisms of BPA on PU MPs that have undergone different aging treatments, and provides a theoretical basis for the assessment of environmental behavior and exposure risks when PU MPs and BPA coexist.