A perfect organic crystal while keeping high quality semiconductor/dielectric interface with minimal defects and disorder is crucial for the realization of high performance organic single crystal field-effect transistors (OSCFETs). However, in most reported OSCFET devices, the crystal transfer processes is extensively used. Therefore, the semiconductor/dielectric interface is inevitably damaged. Carrier traps and scattering centers are brought into the conduction channel, so that the intrinsic high mobility of OSCFET devices is entirely disguised. Here, very thin pentacene single crystal is grown directly on bare SiO2 by developing a 'seed-controlled' pentacene single crystal method. The interface quality is controlled by an in situ fabrication of OSCFETs. The interface is kept intact without any transfer process. Furthermore, we quantitatively analyze the influence of crystal thickness on device performance. With a pristine interface and very thin crystal, we have achieved the highest mobility: 5.7 cm2 V−1 s−1—more than twice the highest ever reported pentacene OSCFET mobility on bare SiO2. This study may provide a universal route for the use of small organic molecules to achieve high performance in lamellar single crystal field-effect devices.