Nanotetragonal　LiYF4:RE　(Tm,Er,Ho)　is　a　kind　of　excellent　upconversion　luminescence　(UCL)　material　potentially　used　in　many　fields,　while　the　enhancement　of　UC　emission　and　regulation　of　luminescence　lifetime　are　still　a　challenge.　Herein,　a　strategy　was　reported　to　enhance　UCL　performance　with　the　aid　of　the　construction　of　a　3Yb-Er-Hf　sublattice　energy　cluster　with　the　introduction　of　H1　and　the　interception　of　surface　defect　fluorescence　quenching.　UCL　was　obviously　decreased　by　Hf4+　doping　without　surface　defect　elimination,　but　after　the　interception　of　surface　defect　quenching,　UCL　was　dramatically　enhanced　more　than　300-fold　with　an　Er3+/Hf4+　mole　ratio　of　1:1.　The　contribution　of　UCL　enhancement　by　the　construction　of　a　3Yb-Er-Hf　sublattice　energy　cluster　is　about　1.5　times　of　the　sample　without　energy　cluster　construction.　Interestingly,　the　lifetime　of　UCL　can　also　be　regulated　by　this　strategy.　According　to　the　results　of　systematical　microstructure　analyses　and　UCL　performance　behaviors　examined　by　X-ray　powder　diffraction　(XRD),　small-angle　X-ray　scattering　(SAXS),　transmission　electron　microscopy　(TEM),　nuclear　magnetic　resonance　(NMR),　and　fluorescence　spectrophotometry　(FS)　methods,　the　possible　mechanism　of　UCL　enhancement　was　proposed.　This　work　may　be　an　inspiration　for　researchers　to　design　and　develop　high-performance　UCL　nanomaterials.