There now exist a handful of solids that exhibit sufficient mobility of Li-ions to be considered viable electrolytes for battery applications. While these are exciting developments, recent research has shown, however, that high ionic mobility is in itself insufficient -- several other properties of a solid electrolyte are essential for use in electrochemical environments. Key amongst these are interfacial properties, which include stabilitiy, charge transport, wettabiity, and elastic properties. This presentation will summarize our recent computational studies of multiple interfacial issues in the promising solid electrolyte, LLZO. A wide range of computational methods are brought to bear on these phenomena; coupling to experimental measurements will be highlighted.