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Detailed understanding of solid–solid interface structure–function relationships is critical for the improvement and wide deployment of all‐solid‐state batteries. The interfaces between lithium phosphorous oxynitride (LiPON) solid electrolyte material and lithium metal anode, and between LiPON and Li  x  CoO 2  cathode, have been reported to generate solid–electrolyte interphase (SEI)‐like products and/or disordered regions. Using electronic structure calculations and crystalline LiPON models, we predict that LiPON models with purely P−N−P backbones are kinetically inert towards lithium at room temperature. In contrast, transfer of oxygen atoms from low‐energy Li  x  CoO 2 (104) surfaces to LiPON is much faster under ambient conditions. The mechanisms of the primary reaction steps, LiPON structural motifs that readily reacts with lithium metal, experimental results on amorphous LiPON to partially corroborate these predictions, and possible mitigation strategies to reduce degradations are discussed. LiPON interfaces are found to be useful case studies for highlighting the importance of kinetics‐controlled processes during battery assembly at moderate processing temperatures.

Kinetics‐Controlled Degradation Reactions at Crystalline LiPON/Li x CoO 2 and Crystalline LiPON/Li‐Metal Interfaces