AbstractBody centered cubic (bcc) Mg–Li‐based alloys are a promising light‐weight structural material. In order to tailor the Mg–Li composition with respect to specific industrial requirements, systematic materials‐design concepts need to be developed and applied. Quantum‐mechanical calculations are increasingly employed when designing new alloys as they accurately predict basic thermodynamic, structural, and functional properties using only the atomic composition as input. We have therefore performed a quantum‐mechanical study using density functional theory (DFT) to systematically explore fundamental physical properties of a broad set of bcc MgLi‐based compounds. These DFT‐determined properties are used to calculate engineering parameters such as (i) the specific Young's modulus (Y/ρ) or (ii) the bulk over shear modulus ratio (B/G) which allow differentiating between brittle and ductile behavior. As we have recently shown, it is not possible to increase both specific Young's modulus, as a measure of strength, and B/G ratio, as a proxy for ductility, by changing only the composition in the binary bcc Mg–Li system. In an attempt to bypass such fundamental materials‐design limitations, a large set of MgLi–X substitutional ternaries derived from stoichiometric MgLi with CsCl structure are studied. Motivated by the fact that for Mg–Li alloys (i) 3rd row Si and Al and (ii) 4th row Zn are industrially used as alloying elements, we probe the alloying performance of the 3rd (Na, Al, Si, P, S, Cl) and 4th row transition metal (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) elements. The studied solutes offer a variety of properties but none is able to simultaneously improve both specific Young's modulus and ductility. Therefore, in order to explore the alloying performance of yet a broader set of solutes, we predict the bulk modulus of MgX and LiX B2‐compounds running over 40 different elements.