In the present work, we propose a coupled immersed interface and grid based particle method to solve two-phase electrohydrodynamic problems in three dimensions. The problem considers a leaky dielectric (weakly conducting) droplet immersed in another leaky dielectric fluid under electric field where the non-homogeneous droplet surface charge effect is taken into account. Due to the mismatch of electrical properties between two fluids, the electric potential satisfying Laplace equation with jump conditions across the droplet surface is coupled with the conservation equation for the surface charge density. Consequently, we first develop a three-dimensional augmented immersed interface method (IIM) which incorporates some known jump conditions naturally along the normal direction and check the desired accuracy. Here, the grid based particle method (GBPM) is used to track the interface by the projection of the neighboring Eulerian grid points so no requirement for stitching of parameterizations nor body fitted moving meshes. Within the leaky dielectric framework, the electric stress can be treated as an interfacial force so that both the surface tension and electric force can be formulated in a unified continuum force in the Navier-Stokes equations. A series of numerical tests have been carefully conducted to illustrate the accuracy and applicability of the present method to simulate droplet electrohydrodynamics. In particular, we investigate the droplet equilibrium dynamics under weak and strong electric fields in detail. It is interesting to find out a chaotic tumbling motion with irregular rotating modes which we believe that is the first numerical verification to the recent experiments.