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One of the major obstacles restricting the wide applications of Mg alloys is their low Young's modulus at ∼45 GPa, which is uncompetitive to Al alloy over 60 GPa. To resolve this issue, we proposed a new strategy of designing ultra-light Mg-Li alloys by employing the microscale compounds in both HCP and BCC grains to achieve high Young's modulus. HCP or BCC alone cannot achieve a high modulus due to the segregation of solutes at the grain boundaries and the formation of brittle intermetallics in the interdendritic region. We designed chemistry that is so perfect to arrest the excess solutes inside the BCC matrix during solidification and engulf pre-solidified rare earth particles by HCP primary grains which have such a lean chemical composition that has almost no segregation. During solution heat treatment, the dissolution of solutes pushes the BCC boundary towards HCP grains by Ostwald ripening (BCC structures are interconnected but the HCP structures are isolated). During low-temperature aging heat treatment, nucleation of HCP structure on the rare earth particles inside the BCC grain is found, degrading the strength. Therefore, a novel Mg-Li-Al-Zn-Y-Mn-Gd (LAZWMV) alloy with a very high modulus was designed which reaches Young's modulus as high as 61.4 GPa. Micro-compounds (AlLi and Al-X) with average equivalent diameters of 3.76 µm and 6.55 µm were quantified in 3D using X-ray computed tomography and nanoindentation tests for establishing the microstructure-modulus correlation. The influence of Li addition on Mg-Mg was calculated by DFT calculations and the mechanism of modulus improvements has been proposed. [Display omitted] • Ultra-light Mg-Li alloy was designed with high strength and high modulus. • Super-high Young's Modulus of 61.4 GPa was first reported for a novel Mg alloy. • Nanoindentation uncovers the principles of modulus increase in Mg-Li alloys. • Quantitative 3D characterization of high modulus phase using XCT prectict alloy properties. • DFT calculation of Mg-Mg bonds explores the effects of heat treatments. [ABSTRACT FROM AUTHOR]