The preferential orientation of the perovskite (PVK) is typically accomplished by manipulation of the mixed cation/halide composition of the solution used for wet processing. However, for PVKs grown by thermal evaporation, this has been rarely addressed. It is unclear how variation in crystal orientation affects the optoelectronic properties of thermally evaporated films, including the charge carrier mobility, lifetime, and trap densities. In this study, we use different intermediate annealing temperatures Tinter between two sequential evaporation cycles to control the Cs0.15FA0.85PbI2.85Br0.15 orientation of the final PVK layer. XRD and 2D-XRD measurements reveal that when using no intermediate annealing primarily the (110) orientation is obtained, while when using Tinter = 100 °C a nearly isotropic orientation is found. Most interestingly for Tinter > 130 °C a highly oriented PVK (100) is formed. We found that although bulk electronic properties like photoconductivity are independent of the preferential orientation, surface related properties differ substantially. The highly oriented PVK (100) exhibits improved photoluminescence in terms of yield and lifetime. In addition, high spatial resolution mappings of the contact potential difference (CPD) as measured by KPFM for the highly oriented PVK show a more homogeneous surface potential distribution than those of the nonoriented PVK. These observations suggest that a highly oriented growth of thermally evaporated PVK is preferred to improve the charge extraction at the device level.@en