This study describes the transfer printing of an Al2O3 gate dielectric for the fabrication of a top-gate MoS2 FET. The transfer printing of the Al2O3 gate dielectric involves the peeling-off process, etching of the sacrificial layer, and stacking on the MoS2. This method eliminates the direct deposition of Al2O3 gate dielectric on fragile MoS2 and provides an abrupt Al2O3/MoS2 interface. The fabricated FET has small hysteresis, low leakage current, a subthreshold slope of 120 mV dec−1, and a carrier mobility of 7.3 cm2 V−1 s−1. The transfer printing approach is applicable to various high-k gate dielectrics and layered materials for constructing functional devices.