The presented approach allows a precise level-by-level adjustment, since in each step the nano-to micro-structure and the mechanical properties can be tuned by the ligands' chemical structure as well as by the conditions during self-assembly and during crosslinking via heat-treatment. This allows a precise control of the overall final structure on each size regime -from the atomic to the macroscale. We further demonstrate the effect of the adjustable multiscale structure by the tunable functional properties of the composite material.