We predict and analyze density-functional theory (DFT) -based structures for the recently isolated Au₄₀(SR)₂₄ cluster. Combining structural information extracted from ligand-exchange reactions, circular dichroism and transmission electron microscopy leads us to propose two families of low-energy structures that have a chiral Au-S framework on the surface. These families have a common geometrical motif where a non-chiral Au₂₆ bi-icosahedral cluster core is protected by 6 RS-Au-SR and 4 RS-Au-SR-Au-SR oligomeric units, analogously to the “Divide and Protectâ€� motif of known clusters Au₂₅(SR)18^-/0, Au₃₈(SR)₂₄ and Au₁₀₂(SR)₄₄. The strongly prolate shape of the proposed Au₂₆ core is supported by transmission electron microscopy. Density-of-state-analysis shows that the electronic structure of Au₄₀(SR)₂₄ can be interpreted in terms of a dimer of two 8-electron superatoms, where the 8 shell electrons are localized at the two icosahedral halves of the metal core. The calculated optical and chiroptical characteristics of the optimal chiral structure are in a fair agreement with the reported data for Au₄₀(SR)₂₄.