This study explores the efficient decolorization and complete mineralization of the diazo dye Evans blue, using an integrated aerobic bioreactor system coupled with a double-chamber microbial fuel cell (DCMFC) including a bio-cathode and acetate as a cosubstrate. The research addresses the environmental challenges posed by dye-laden industrial effluents, focusing on achieving high decolorization efficiency and understanding the microbial communities involved. The study utilized mixed strains of actinomycetes, isolated from garden compost, to treat initial dye concentrations of 100 mg/L and 200 mg/L. Decolorization efficiency and microbial community composition were evaluated using 16S rRNA sequencing, and electrochemical impedance spectroscopy (EIS) was used to assess anode and DCMFC resistance. The results demonstrated decolorization efficiencies ranging from 90 ± 2% to 98 ± 1.9% for 100 mg/L and from 79 ± 2% to 87% ± 1% for 200 mg/L. An anode resistance of 12.48 Ω indicated a well-developed biofilm and enhanced electron transfer. The microbial community analysis revealed a significant presence of Pseudomonadota (45.5% in dye-acclimated cultures and 32% in inoculum cultures), with key genera including Actinomarinicola (13.75%), Thermochromatium (4.82%), and Geobacter (4.52%). This study highlights the potential of the integrated DCMFC–aerobic system, utilizing mixed actinomycetes strains, for the effective treatment of industrial dye effluents, offering both environmental and bioenergy benefits.