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Pentacene is a key organic semiconductor, which has achieved prominence in transistor applications and as an archetypal material for singlet fission, the process whereby the absorption of one photon leads to the formation of two triplet states. Functional properties of molecules are highly anisotropic, and control over the molecular orientation in thin films with structural templating is commonly implemented as a route for governing the morphology and structure of organic films. Among the structural templating layers, 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA) and copper(I) iodide (CuI) have been shown to effectively template aromatic systems such as phthalocyanines. Here, we extend their use to pentacene thin films and find that a successful transition to a flat-lying arrangement is achieved with CuI films grown at high temperatures, but not with PTCDA. As a result, we postulate a model based on …