The　properties　of　ZnO　single　crystals　irradiated　by　a　pulsed　248　nm　excimer　laser　have　been　systematically　studied　by　XRD,　PL　and　Raman　measurements.　It　was　observed　that　the　surface　roughness　and　the　magnitude　of　the　grain　size　on　the　surface　of　the　irradiated　ZnO　crystals　became　larger,　as　well　as　their　band-edge　emissions　at　room　temperature　were　found　to　become　weaker　and　shift　to　higher　frequency　with　increasing　laser　energy　densities.　Green　luminescence　emission　has　a　contrary　trend.　Our　Raman　results　show　that　bulk　properties　of　the　irradiated　ZnO　crystal　diminish　but　the　defect-,　surface-related　features　display　as　laser　energy　densities　increases.　The　Raman　spectra　of　the　irradiated　ZnO　crystals　are　deteriorated　bulk　spectra　with　spectroscopic　line　broadening　and　merging,　line　intensity　is　reducing,　and　position　shifting,　because　the　laser　irradiation　onto　the　surface　of　ZnO　crystal　leads　to　the　thermal　decomposition　of　ZnO　into　metallic　Zn　and　oxygen　gas　and　the　increase　of　oxygen　vacancies　or　interstitial　Zn　atoms.　A　new　phonon　around　568cm-1　related　to　interstitial　Zn　atoms　in　the　irradiated　ZnO　crystal　was　observed.　These　results　are　associated　with　micro-structure　variation　of　ZnO　single　crystals　caused　by　laser　irradiation.