How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest for centuries. Recently, it has re-emerged as a critical question in a subdiscipline of chemistry - electrochemistry at heterointerphases, where the answers have implications for both how, and in what forms, humanity stores the rising quantities of renewable electric power generated from solar and wind installations world-wide. Here we consider the relation between the surface chemistry at such interphases and the reversibility of electrochemical transformations at a rechargeable battery electrode. Conventional wisdom holds that stronger chemical interaction between the metal deposits and electrode promotes reversibility. We report instead that a moderate strength of chemical interaction between the deposit and the substrate, neither too weak nor too strong, enables highest reversibility and stability of the plating/stripping redox processes at a battery anode. ... : accepted at Science Advances, in press ...