Non-volatile memories based on phase-change materials have gained ground for applications in analog in-memory computing. Nonetheless, non-idealities inherent to the material result in device resistance variations that impair the achievable numerical precision. Projected-type phase-change memory devices reduce these non-idealities. In a projected phase-change memory, the phase-change storage mechanism is decoupled from the information retrieval process by using projection of the phase-change material’s phase configuration onto a projection liner. It has been suggested that the interface resistance between the phase-change material and the projection liner is an important parameter that dictates the efficacy of the projection. In this work, we establish a metrology framework to assess and understand the relevant the structural properties of the interfaces in thin films contained in projected memory devices. Using X-ray reflectivity, X-ray diffraction and transmission electron microscopy, we investigate the quality of the interfaces and the layers’ properties. Using demonstrator examples of Sb and Sb2Te3 phase-change materials, new deposition routes as well as stack designs are proposed to enhance the phase-change material to a projection-liner interface and the robustness of material stacks in the devices.