Existing technology to construct high-temperature superconductor (HTSC) multichip modules (MCM’s) incorporating several YBa2Cu3O7−δ (YBCO) thin films and thick dielectric layers are based on epitaxial growth of all layers from the template of a single-crystal substrate. This work demonstrates an alternate method to fabricate these structures: the use of a biaxially aligned yttria-stabilized zirconia (YSZ) intermediate layer deposited by ion-assisted pulsed-laser deposition. Using this technique, a YBCO thin film with Tc∼87 K and Jc∼3×105 A/cm2 was grown on a 5 μm amorphous SiO2 layer. In addition, YBCO/YSZ/SiO2/YSZ/YBCO/CeO2/YSZ and YBCO/YSZ/amorphous-YSZ/YBCO/CeO2/YBCO multilayer structures were constructed.