Semiconductor metal oxide materials have gained huge attention in gas sensors owing to their high sensitivity to many target gases. Herein, ZnO/CuO core-shell and ZnO/CuO hybrid, which were synthesized by different sol-gel methods and formed in two different crystal structures, were used as an additive material to enhance the response range of 8-hydroxypyrene-1, 3, 6-trisulfonic acid (HPTS) for the sensing of gaseous carbon dioxide. Metal oxide materials were characterized by using XPS, XRD, FTIR, SEM, UV-Vis, and PL spectroscopy. The HPTS dye along with the ZnO/CuO hybrid material displayed a higher CO2 gas sensitivity as 94% ratio (I0/I100=16.90) and Stern-Volmer constant (KSV) value and extended linear response range compared to the HPTS-based sensing thin films along with ZnO/CuO coreshell material and additive-free form. ZnO/CuO core-shell and hybrid structures were used for enhancing of carbon dioxide sensitivity of the HPTS dye.