Natural zeolite (NZ) offers unique surface properties that enable its use in environmental remediation and catalytic applications. In this study, a graphene oxide/natural zeolite/bismuth oxide (GO/NZ/Bi₂O₃) composite was developed to enhance the functional performance of NZ for the photocatalytic degradation process relevant to environmental treatment. The composite was synthesized through a two-step calcination process: NZ was first calcined with bismuth oxide (Bi₂O₃) at 900 °C to form the NZ/Bi₂O₃ composite, followed by graphene oxide (GO) incorporation and a secondary calcination at 300 °C. Structural characterization revealed apatite-type and eulytite mineral phases in the NZ/Bi₂O₃ system, reflecting phase transformations arising from high-temperature interaction between NZ and Bi₂O₃. Incorporation of GO resulted in a dominant calcium bismuth oxy-silicate phase. FTIR spectra confirmed characteristic Si–O–Si and Si–O–Al vibrations inherent to natural zeolite, alongside Bi–O and C–O bands indicative of successful composite formation. SEM analyses showed porous NZ structures supporting agglomerated Bi₂O₃ particles and irregular GO flakes, while TGA-DTG identified thermal events associated with moisture release, NZ-bound water, GO degradation, and Bi₂O₃ transitions. BET measurements exhibited a Type IV isotherm and a surface area of 1.06 m²/g, consistent with mesoporous mineral composites. Zeta potential data revealed reduced suspension stability following GO integration. Notably, the GO/NZ/Bi₂O₃ composite demonstrated superior photocatalytic degradation efficiency, underscoring the enhanced reactivity achieved through synergistic modification of natural zeolite. Overall, this work highlights the geochemical adaptability of natural zeolite and its potential for advanced environmental applications.