The biodegradation of polyurethane foam (PU foam) using a combination of oxidative pre-treatment (ozonization) and Tenebrio molitor (T. molitor) mealworms was conducted in this study. Different degrees of ozone oxidation (0%, 25%, and 50%) were applied to PU foam, which was subsequently fed to mealworms. The mealworms' survival and growth were then compared to mealworms receiving a normal diet (bran). Results showed that mealworms fed with non-oxidized PU foam (PUF0) exhibited a higher consumption rate (11.8%) than those fed with 25% (PUF25) and 50% (PUF50) oxidized PU foam (7.7% and 5.7%, respectively). The survival rate was similar across all the PU foam diets and the bran diet. Fourier transform infrared (FTIR) spectroscopy and differential scanning calorimetry (DSC) analyses revealed minor structural changes in the PU foam. The gut microbiota analysis showed a significant correlation between the PU foam and bran diets. Among the different oxidized PU, distinct microbial community profiles were also observed, with the genus Klebsiella consistently present across the PU foam diets. The ozone pre-treatment altered the palatability and degradation of the PU foam by mealworms, while the mealworm frass and chitin obtained could potentially be used as resources for agricultural and industrial applications that would close the circular bio-economy cycle.