Biocorrosion and biodegradation behavior of Mg–4Li–1Ca alloy were investigated for industrially important end product conditions, namely the homogenized, rolled, and rolled + annealed ones. Among the three, homogenized material showed the highest corrosion rate (27.2 mm/year) in a simulated body fluid (SBF) owing to its coarse grain structure containing long dumbbell-shaped eutectic phase. Rolled? annealed material exhibited the lowest corrosion rate (0.94 mm/year) corresponding to the highest corrosion resistance (1.854 kΩ cm2) in SBF. This higher corrosion resistance is associated with a uniform distribution of corrosion sites and a lower occurrence of twins in the microstructure. However, the rolled material showed a greater corrosion rate due to an appreciable volume fraction of {1011} compression twins, {1012} tension twins, and {1011}–{1012} double twins, which form galvanic couples with the adjacent grains that enhances localized corrosion. A mechanism of biodegradation at the alloy/SBF interface is proposed. It involves the formation of bone-like hydroxyapatite and metastable octa calcium phosphate, along with other degradation products, such as magnesium hydroxide and lithium hydroxide. © Springer Science+Business Media New York 2015.