Iridium nanoparticles were synthesized between graphite layers by thermal treatment of the mixture of iridium chloride (IV) and graphite powder under chlorine atmosphere followed by hydrogen reduction (Ir-GIC). In Ir-GIC samples with 1–6 wt% iridium metal loadings, all iridium nanoparticles with disk-shape (iridium nanodisks) were located between graphite layers; however, iridium nanoparticles on graphite surface were also formed in addition to iridium nanodisks in the Ir-GIC samples with 8 and 10 wt% iridium metal loadings. Iridium nanodisks between graphite layers were highly active for cinnamaldehyde hydrogenation and selective to cinnamyl alcohol compared with the iridium particles on graphite surfaces.