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The combination (AIM-ME) of atomic layer deposition in metal-organic frameworks (MOFs) and metal exchange (ME) is introduced as a technique to install dispersed metal atoms into the mesoporous MOF, NU-1000. Zn-AIM, which contains four Zn atoms per Zr6 node, has been synthesized through AIM and further characterized through density functional calculations to provide insight into the possible structure. Zn-AIM was then subjected to modification via transmetalation to yield uniform porous materials that present nonstructural Cu, Co, or Ni atoms. (Figure Presented).