Alargediamondcrystalupto500μmindiameterwithasmooth(100)facetatitstophasbeensynthesizedonMosubstratethroughmicrowaveplasmachemicalvapordeposition(MPCVD).Itsmorphologyandqualitywerecharacterizedbyscanningelectronmicroscopy(SEM),andthegrowthmechanismwasroughlyillustratedfrombothmacroscopicandmicroscopicviewpoints.Itwasfoundthatmorphologicalinstabilitiesareamajorfactorresultinginsynthesisoflargediamondcrystals,moreover,highmicrowavepowerdensity(MPD),highCH4concentrations,highpressure,highsubstratesurfacetemperatureandtheadditionofasmallamountofO2werealsonecessaryforthesynthesisoflargediamondcrystals.