Using　ultrathin　alumina　membranes　(UTAMs)　as　evaporation　or　etching　masks　large-scale　ordered　arrays　of　surface　nanostructures　can　be　synthesized　on　substrates.　However,　it　is　a　challenge　for　this　technique　to　synthesize　quantum-sized　surface　structures.　Here　an　innovative　approach　to　prepare　UTAMs　with　regularly　arrayed　pores　in　the　quantum　size　range　is　reported.　This　new　approach　is　based　on　a　well-controlled　pore-opening　process　and　a　modulated　anodization　process.　Using　UTAMs　with　quantum-sized　pores　for　the　surface　patterning　process,　ordered　arrays　of　quantum　dots　are　synthesized　on　silicon　substrates.　This　is　the　first　time　in　realizing　large-scale　regularly　arrayed　surface　structures　in　the　quantum　size　range　using　the　UTAM　technique,　which　is　an　important　breakthrough　in　the　field　of　surface　nanopatterning.