The purpose of this study was to investigate the friction and wear behavior of single crystal superalloys at elevated temperatures. Pin-on-plate experiments were conducted using a custom-built high-temperature fretting/wear apparatus. Measurements were performed on two single crystal Ni-based alloys and Waspaloy® (used as a baseline material). The coefficient of friction for the single crystal materials (i.e., during running-in and steady state) was lower compared to the Waspaloy®. In addition, the experiments showed that the friction coefficient of the single crystal is dependent on the crystallographic plane; the friction coefficient was lower for the tests on the {100} plane compared to the {111} plane. The wear behavior was aligned with the friction behavior, where the single crystal Ni-based alloys showed slightly higher wear resistance compared to the Waspaloy®. Ex situ analysis by means of FIB/SEM and XPS analysis revealed the formation of Co-base metal oxide layer on the surface of the single crystal alloy. Similarly, a Co-base oxide layer is observed on the counterface providing a self-mated oxide-on-oxide contact and thus lower friction and wear compared to the Waspaloy®.