X-ray charge densities of Al-based icosahedral quasicrystalline approximant crystals $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlReSi},$ $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlMnSi},$ and ${\mathrm{Al}}_{12}\mathrm{Re}$ were observed by a combination of the maximum entropy method with the Rietveld method. We successfully obtained the clear images of interatomic covalent bonds between Al and transition metals (Mn, Re) and those in the Al (or Si) icosahedron in Mackay icosahedral clusters of both $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlReSi}$ and $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlMnSi}$ approximant crystals. The bonding nature of the three kinds of glue atom sites connecting Mackay icosahedral clusters was also clarified. This covalent bonding nature should strongly relate with the enhancement of the electron density-of-states pseudogap near the Fermi level. In addition, the interatomic covalent bonds of $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlReSi}$ are stronger than those of $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlMnSi}.$ This fact leads to the low effective carrier density of $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlReSi}$ in comparison with that of $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlMnSi}.$ Unlike the covalent bonding nature of an icosahedron in $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlReSi}$ and $\ensuremath{\alpha}\ensuremath{-}\mathrm{AlMnSi}$ crystals, the Al icosahedron with an Re center atom exhibits no Al-Al interatomic covalent bonds in the ${\mathrm{Al}}_{12}\mathrm{Re}$ crystal. The tendency for metallic-covalent bonding conversion in the Al icosahedron, which is related to the atom site occupancy of the icosahedral cluster center, is also strongly supported.