Transient materials are an emerging class of materials that are designed to undergo disintegration at a predefined rate and a predefined manner. Transient materials are utilized in structures and devices to enable device transiency, in particular, transient electronics. While interfacial stress in layered structures is well studied and—to a large extent—well understood, the same in transient layered structures remains a challenging matter to study and understand. This is solely because of the dynamic chemical and physical properties of the transient materials as well as swelling‐induced stress that is introduced to the interface due to the mismatch in physical properties of the dissimilar materials forming layers. In this work, interfacial interactions of a particular case of polymeric substrate with lithium titanate electrode coating layer are studied and reported. The structure is analogous to that of the anode in a type of lithium‐ion batteries; yet, it can be extended to more general cases of soft electronics. This coordinated experimental–analytical simulation study exhibits formation, accumulation, and propagation of swelling‐induced stress through the membrane‐coating interface, when in transient mode. Swelling‐induced stress as a function of electrode thickness is studied; the analytical data and simulations are verified by experimental results. The stress analysis method can be extended to analyze interfacial stress in a wide range of layered structures with dynamic properties.