Organic semiconductors have been receiving intensive attention due to the specific advantages of low-temperature processing ability, low-fabrication cost, flexibility, and so forth. The charge carrier mobility of higher than 10 cm 2 V −1 s −1 for organic semiconductors is of great importance to be studied since it presents a future promising research direction toward commercial microelectronic applications. With the significant progress of the discovery of novel organic molecules and the further improvements of device fabrication technology, some organic molecules can break the limit of our knowledge and show very high mobilities. In this review, organic polymers and small molecules with mobilities above 10 cm 2 V −1 s −1 are first introduced to provide the readers with a general understanding of the features and characteristics of high-performance organic semiconductors. Then, some important parameters, including the molecular structures, the device configurations, and the performance, are discussed in detail. Finally, the clues to obtain high mobility are summarized, and the perspective toward the future possible research directions are also provided.