The challenges and research needs for the interface engineering of thin-film solar cells using inorganic-compound semiconductors are discussed from a materials-science point of view. It is, in principle, easily possible to define optimized device structures from physical considerations. However, to realize these structures, many materials' limitations must be overcome by complex processing strategies. In this paper, interface properties and growth morphology are discussed using CdTe solar cells as an example. The need for a better fundamental understanding of cause–effect relationships for improving thin-film solar cells is emphasized.