This study revealed the feasibility of simultaneous bioelectricity generation and dye decolorization (SBG&DD) of microbial fuel cells (MFCs) in salty media. With supplementation of decolorized intermediates (DIs), MFCs significantly enhanced the performance of SBG&DD. Due to supplementation of DIs, electron-transporting characteristics of microbes effectively increased the electron-transfer flux in MFCs. By adding various species of DIs at different levels, optimal stimulation of DIs to SBG&DD could be achieved. This also significantly increased color removal efficiencies. Apparently, DI-augmented MFCassisted bioremediation seemed to be the most promising strategy to resolve operation disadvantages of dye decontamination in salty media. The approach provided effective alternatives to improve decolorization of textile dyes and suggested strategies for bioremediation of recalcitrant organics.