Unexpected Ge–Ge interactions were found in “two‐dimensional” Ge4Se3Te as reported by R. Dronskowski et al. in their Communication on page 10204 ff. The layered material was crystallized using chemical vapor deposition and then characterized for the first time. Its electronic structure and the chemical cause of the Ge–Ge interactions were examined by chemical bonding analysis and the newly introduced density of energy (DOE) function.