Landfill leachate nanofiltration concentrate is a kind of wastewater containing high concentrations of color and refractory organics. Herein, we proposed a novel three-dimensional electrochemical technology (3DET) with waste aluminum scraps as particle electrodes for its treatment. The planar and particle electrodes were first optimized. Ti/RuO2 and graphite were used as anodes in the two-dimensional electrochemical technology (2DET). In the light of contaminant removal (color, UV254, COD, and TOC), chlorine reduction, and energy consumption, graphite was selected as planar anodes and cathodes. Moreover, 3DET with Al particle electrodes (Al 3DET) outperformed that with conventional granular activated carbon electrodes, 2DET, and Al particles. At 120 min, the removal efficiencies of color, UV254, COD, and TOC using Al 3DET were 98.94 %, 84.72 %, 51.93 %, and 67.46 %, respectively. UV–vis and EEM spectroscopy, and GC–MS analyses indicate that macromolecular organic matter such as humic-like substances could be effectively degraded and simultaneously removed. Reactive species identification tests including free radical quenching and EPR spectra were conducted. The results indicate that in addition to anodic direct oxidation, indirect oxidation by oxidative species (H2O2, •OH, and RCS) and flocculation by Al species also played a vital role in contaminant removal. Continuous-flow experiments show that Fe EC as a post-treatment step of Al 3DET could effectively provide a neutralization effect for the 3DET effluent and enhance the removal efficiency of contaminants. The total operating cost of combined process was 1.307 USD/m3. This study shows that the Al 3DET-Fe EC process is a promising technology for the treatment of nanofiltration concentrate.