We show that interlayer charge transfer in 2D materials can be driven by an in-plane electric field, giving rise to electrical multipole generation in linear and second order in-plane field. The linear and nonlinear effects have quantum geometric origins in the Berry curvature and quantum metric, respectively, defined in extended parameter spaces characteristic of layered materials. We elucidate their symmetry characters and demonstrate sizable dipole and quadrupole polarizations, respectively, in twisted bilayers and trilayers of transition metal dichalcogenides. Furthermore, we show that this effect is strongly enhanced during the topological phase transition tuned by interlayer translation. The effects point to a new electric control on the layer quantum degree of freedom.