Confined low dimensional charges with high density such as two-dimensional electron gas (2DEG) at interfaces and charged domain walls in ferroelectrics show great potential to serve as functional elements in future nanoelectronics.However,stabilization and control of low dimensional charges is challenging,as they are usually subject to enormous depolarization fields.Here,we demonstrate a method to fabricate tunable charged interfaces with ～77°,86° and 94° head-to-head polarization configurations in multiferroic BiFeO3 thin films by grain boundary engineering.The adjacent grains are cohesively bonded and the boundary is about 1 nm in width and devoid of any amorphous region.Remarkably,the polarization remains almost unchanged near the grain boundaries,indicating the polarization charges are well compensated,i.e.,there should be two-dimensional charge gas confined at grain boundaries.Adjusting the tilt angle of the grain boundaries enables tuning the angle of polarization configurations from 71° to 109°,which in turn allows the control of charge density at the grain boundaries.This general and feasible method opens new doors for the application of charged interfaces in next generation nanoelectronics.