Iridium nanoparticles (IrNPs) and submicroparticles (IrSMPs) with different shapes were synthesized and assembled on indium thin oxide (ITO) and Si substrates using two different methods: direct surface growth and drop-drying assembly. The obtained IrNPs and IrSMPs were characterized using scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS). The IrSMPs (or IrNPs) with disc-like shape and irregular shapes were obtained on ITO substrate by direct surface growth method using polyvinylpyrrolidone (PVP) and sodium citrate as different stabilizers, respectively. The reaction time and the injection temperature of reducing agent are found to have great effect on the size and morphology of the surface-grown Ir particles. The disc-like, ellipsoidal, and spherical IrSMPs (or IrNPs) were also synthesized in homogeneous solution in the presence of H3BO3 and Na2B4O7 as assistant-stabilizer. These IrNPs and IrSMPs were used as building blocks to construct nanoparticle assemblies by using a simple drop-drying method. Uniform IrNP and IrSMP assemblies were successfully prepared on Si and ITO substrates, indicating that the drop-drying method is efficient for the preparation of not only nanoparticle assemblies but also submicroparticle assemblies.