The　original　motivation　of　the　article　is　to　give　a　systematic　investigation　on　the　protocol　of　combining　computer　simulation　and　accurate　synthesis　of　serial　peptide　protected　gold　clusters　for　potent　tumor　targeting　therapy.　Glutathione　peroxidase-1　(GPx-1)　is　a　crucial　antioxidant　selenoenzyme　that　regulates　cellular　redox　level,　thus　becomes　a　potential　target　in　cancer　treatment.　We　firstly　utilize　molecular　dynamic　(　MD)　simulation　to　rationally　design　and　screen　serial　peptide-Au　cluster　compounds　with　special　peptide　sequences　and　precise　gold　atoms,　which　can　recognize　and　bind　specific　domain　of　GPx-1　with　high　affinity.　The　theoretical　simulations　were　further　verified　by　the　following　peptide-Au　clusters　synthesis　and　GPx-1　activity　suppression　studies　in　buffer　and　cells,　respectively.　Further　cytological　experiments　corroborated　that　peptide-Au　clusters　are　promising　nanoparticles　inducing　tumor　cells　apoptosis　by　suppressing　GPx-1　activity　and　increasing　higher　cellular　reactive　oxygen　species　level　to　initiate　tumor　cell　apoptosis　through　intrinsic　mitochondrial　pathway.