Ion bombardment on the surface of a substrate during deposition of a thin film [ion-assisted (IA) deposition] is used to control thin-film crystalline orientation and phase. Ion-assisted deposition is demonstrated with the relatively new pulsed-laser deposition (PLD) technique, a method of thin-film growth that has shown promise for the synthesis of high-temperature superconductor and other complex oxide films. A versatile vacuum chamber with independent control of ion-gun parameters was developed for ion-assisted pulsed-laser deposition (IAPLD). Control of crystalline orientation and alignment of yttria-stabilized zirconia and CeO2 layers for use in YBa2Cu3O7−δ superconductor devices is demonstrated using this IAPLD technology.