This study presents a novel approach for fabricating ZIF-8 membranes supported on α-alumina hollow fibers through the introduction of a graphene oxide (GO) gutter layer and the application of zinc oxide (ZnO) Atomic Layer Deposition (ALD). The method successfully addressed key challenges, including excessive precursor penetration and membrane thickness. The introduction of the GO layer and subsequent ZnO ALD treatment significantly reduced membrane thickness to approximately 300 nm and eliminated delamination issues between the GO layer and the alumina support. The optimized membranes demonstrated enhanced propylene permeance, with values approximately three times higher than those of membranes without GO, and achieved higher separation factors, indicating minimal inter-crystalline defects. Notably, the GO layer influenced the microstructure, leading to an increase in permeance with rising temperatures. These findings highlight the potential of this strategy for developing high-performance ZIF-8 membranes for gas separation applications.