We were first to synthesize the Zr metal-organic framework (MOF), UiO-66 (Zr6O4(OH)(4)(BDC)(6); BDC: 1,4-benzenedicarboxylate) by a seed-mediated spray-drying method. Furthermore, a pillared-layer-type MOF, CID-1 ([Zn-2(ip)(2)(bpy)(2)]; ip: isophthalate, bpy: 4,4'-bipyridine) was also synthesized successfully. This is the first demonstration of a spray-drying synthesis of an MOF consisting of two kinds of ligands.