Halogen ions (I(-), Br(-), Cl(-)) were added into a colloidal solution of CdSe and PbS quantum dots (QDs) to form QDs capped with these inorganic ligands. Halogen ions attached to QDs through electrostatic interactions and the varying coordination strength between the inorganic ligands and QDs led to different degrees of redispersion and stabilization in polar solvents. Moreover, we successfully conducted electrophoretic deposition (EPD) of QDs capped with inorganic ligands. Negatively charged QDs were adsorbed onto a positively charged TiO2 anode. The assembled QDs films were used in photovoltaic devices and offered better efficiency than QDs capped with organic ligands. This work demonstrates that halogen ions are indeed promising ligands to improve the stability of QDs with inorganic ligands and the EPD method shows prospects in assembling QDs films for practical applications.