Hierarchical heteronuclear metal-organic gels (MOGs) based on iron (Fe) and aluminium (Al) metal-organic framework (MOF) backbones bridged by tri-carboxylate ligands have firstly been synthesized by simple solvothermal method. Monometallic MOGs based on Fe or Al give homogenous monoliths, which have been tuned by introduction of heterogeneity in the system (mismatched growth). The developed gels demonstrate that surface areas, pore volumes and pore sizes can be readily tuned by optimizing heterogeneity. The work also elaborates effect of heterogeneity on size of MOG particles which increase substantially with increasing heterogeneity as well as obtaining mixed valence sites in the gels. High surface areas (1861m2/g) and pore volumes (9.737cc/g) were obtained for heterogeneous gels (0.5Fe-0.5Al). The large uptakes of dye molecules (290mg/g rhodamine B and 265mg/g methyl orange) with fast sorption kinetics in both neutral and acidic mediums show good stability and accessibility of MOG channels (micro and meso-/macropores), further demonstrating their potential applications in catalysis and sorption of large molecules.