In this article, an effective way of chemical modification on the dielectric surface (Al 2 O 3 ) is investigated to chemical vapor deposition (CVD)-grown high-quality monolayer MoS 2 and the relevant back-gated FETs are fabricated without MoS 2 transfer. As a result, the size of the triangle MoS 2 is increased and its quality is improved as the surface of Al 2 O 3 is treated by H 2 SO 4 . Furthermore, as compared with the gate dielectrics of the SiO 2 and as-deposited Al 2 O 3 , the fabricated transistor with the H 2 SO 4 -treated Al 2 O 3 as gate dielectric achieves better electrical properties: high carrier mobility of 12.9 cm 2 /Vs (~10 times higher than the untreated sample, ~5.2 times higher than the SiO 2 gate-dielectric sample), small subthreshold swing of 110 mV/dec, and high ON/OFF ratio of 3 × 10 6 . The involved mechanisms are attributed to the fact that the H 2 SO 4 -treated Al 2 O 3 not only can increase its surface roughness to promote the nucleation and high-quality growth of MoS 2 but also can improve the quality of the MoS 2 /Al 2 O 3 interface. This simple chemical-modification treatment will open up an effective approach of combining the high-crystallinity CVD-MoS 2 with the high-k dielectric without MoS 2 transfer required.