The coexistence of large particles (such as biomass or coal particles) and fine particles in gas-solid flow is common. In this study, an Eulerian-Lagrangian-Lagrangian method (EMMS-DPM-DEM) was developed to simulate the binary gas-solid flow containing particles of significantly different sizes, where fine particles were simulated using coarse grained discrete element method and the motion of large particles was captured using discrete element method. Experiments on density segregation of large particles were also carried out to validate the developed simulation method. It was shown that EMMS-DPM-DEM can predict the density segregation process of large particles reasonably well. Furthermore, the density segregation mechanism of large particles in a dense fluidized bed was explained at different scales, i.e., the Archimedes principle at macroscale, the entrainment and the global circulation pattern due to bubble motions at mesoscale and the particle-particle and gas-particle interactions at microscale. The method proposed here can be directly used to study the hydrodynamics of biomass thermochemical conversion in fluidized beds, although it was validated using segregation experiments of coal particles. (C) 2019 Elsevier Ltd. All rights reserved.