Herein,　a　mechanism　of　stepwise　metal-center　exchange　for　a　specific　metal-organic　framework,　namely,　[Zn-4(dcpp)(2)(DMF)(3)(H2O)(2)](n)　(H(4)dcpp=4,5-bis(4-carboxylphenyl)phthalic　acid),　is　disclosed　for　the　first　time.　The　coordination　stabilities　between　the　central　metal　atoms　and　the　ligands　as　well　as　the　coordination　geometry　are　considered　to　be　dominant　factors　in　this　stepwise　exchange　mechanism.　A　new　magnetic　analytical　method　and　a　theoretical　model　confirmed　that　the　exchange　mechanism　is　reasonable.　When　the　metathesis　reaction　occurs　between　Cu-II　ions　and　framework　Zn-II　ions,　the　magnetic　exchange　interaction　of　each　pair　of　Cu-II　centers　gradually　strengthens　with　increasing　amount　of　framework　Cu-II　ions.　By　analyzing　the　changes　of　coupling　constants　in　the　Cu-exchanged　products,　it　was　deduced　that　Zn4　and　Zn3　are　initially　replaced,　and　then　Zn1　and　Zn2　are　replaced　later.　The　theoretical　calculation　further　verified　that　Zn4　is　replaced　first,　Zn3　next,　then　Zn1　and　Zn2　last,　and　the　coordination　stability　dominates　the　Cu/Zn　exchange　process.　For　the　Ni/Zn　and　Co/Zn　exchange　processes,　besides　the　coordination　stability,　the　preferred　coordination　geometry　was　also　considered　in　the　stepwise-exchange　behavior.　As　Ni-II　and　Co-II　ions　especially　favor　octahedral　coordination　geometry　in　oxygen-ligand　fields,　Ni-II　ions　and　Co-II　ions　could　only　selectively　exchange　with　the　octahedral　Zn-II　ions,　as　was　also　confirmed　by　the　experimental　results.　The　stepwise　metal-exchange　process　occurs　in　a　single　crystal-to-single　crystal　fashion.