A bifunctional catalyst, comprising GaZr oxide and SAPO-34 zeolite, manifests enhanced catalytic activity in CO₂ hydrogenation to light olefins; nonetheless, the comprehensive analysis of the pivotal role played by the underlying structure of ZrO₂ in Ga-Zr oxide has not been investigated. Herein, different crystalline structures of ZrO₂ were prepared by the co-precipitation method and adopted as a support to deposit Ga to obtain ZrO₂ with different ratios of monoclinic ZrO₂ (m-ZrO₂) to tetragonal ZrO₂ (t-ZrO₂) in GaZr oxides for CO₂ hydrogenation to light olefins. Various characterizations demonstrated that the interface between Ga and the mixed phase of (m-t) ZrO₂ produces more oxygen vacancies which favors the adsorption and activation of CO₂, and the larger specific surface area and stronger H₂ adsorption and dissociation capacity promote CO₂ conversion. Interestingly, the GaZr oxide with high m-ZrO₂ content exhibits superior catalytic activity than the GaZr oxide with high content of t-ZrO₂. The highest light olefins yield (9.0%) and selectivity (77.9%) (CO free) with 27.9% CO₂ conversion was achieved. In-situ DRIFT spectra further elaborated that the GaZr oxides with different ZrO₂ crystalline phases follow the same reaction pathway to hydrogenate CO₂ first to HCOO* and then to CH₃O* on GaZr oxide surface. While compared with sole ZrO₂, the introduction of Ga significantly promotes the hydrogenation of HCOO* to CH₃O*, acting as a crucial reaction intermediate that subsequently diffuses into SAPO-34 pores to enhance the desired light olefins selectivity.