The domain structure, dielectric, and piezoelectric properties of 0.7 Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-PT) single crystals with nanocomposite electrode, which includes MnOx semiconductor nanogratings and a Ti/Au conductive layer, were studied in this paper. These artificial MnOx nanogratings can alter the electric field distribution and then enhance the domain density. PMN-PT crystals with Ti/Au-MnOx nanocomposite electrodes showed high piezoelectric constant of 2250 p.m./V and dielectric constant of 5400 at 1 kHz, respectively. Compared to ones with conventional planar electrodes, the piezoelectric and dielectric constants of the samples with nanocomposite electrodes were increased 36.7% and 38.3%, respectively. Piezoresponse force microscopy (PFM) images revealed the domain pattern near the electrode/single crystal interface. A linear domain structure induced by the MnOx nanocomposite electrode was found in the samples with thickness less than 200 μm. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) results showed the diffusion of Mn about 300 nm in depth in PMNPT crystal after heat treatment during MnOx nanocomposite electrode. It is believed that the localized high electric fields induced by fringe effects caused by the nanocomposite electrode can enhance nucleation of new domains, and that diffusion from the patterned Mn layer may also lead to an enhancement in domain wall mobility. Our findings open up a new domain engineering technique for tailoring the dielectric and piezoelectric properties of PMN-PT single crystals.