Electric field-induced particle polarization is essential to the electro-responsive electrorheological (ER) effect of particle suspensions. In this work, we use graphene oxide (GO) as a soft and polar coating shell to prepare GO-wrapped titania dielectric microspheres for use as the dispersal phase of an ER suspension. Under a DC electric field, the ER characteristic of GO-wrapped titania microspheres dispersed in silicone oil is investigated by rheological tests, and then compared with that of a suspension of bare titania microspheres. The results show that the suspension of GO-wrapped titania microspheres possesses an enhanced ER characteristic. Its field-induced shear yield stress and storage modulus are much higher than those of the suspension of bare titania microspheres. The soft and polar GO shell is regarded as the origin of the ER enhancement. Dielectric analysis indicates that wrapping GO can enhance the interfacial polarization and thus improve the ER characteristics of titania microspheres. Wrapping GO onto the surface of titania microspheres can also reduce the particle sedimentation velocity of the suspension.