Herein, ternary composites from polypyrrole (PPy), Mn0.8Zn0.2Fe2O4 (MZF), and graphite oxide (GO) were prepared to remove acid red dye (AR1) from wastewater. MZF was synthesized using spent Zn–C batteries, acid leaching, and sucrose auto-combustion processes; GO was prepared via oxidation and exfoliation of graphite. The composites were prepared by adding MZF and GO during the in-situ polymerization of pyrrole. Different PPy/MZF/GO (PMG) composites were prepared by changing the weight ratios of the PPy, MZF, and GO. We investigated the prepared composites’ structural, magnetic, and electrical/dielectric properties. We evaluated different experimental conditions’ influences on dye removal performance, such as pH, dosage, dye concentration, temperature, and contact time. XRD, FT-IR, and magnetic properties indicated that PPy completely coated the other contents. The electrical/dielectric properties improved while increasing the GO ratio. The PMG at GO content 50 wt.% (PMG50) showed the most efficient ratio for better removing AR1 from wastewater.