you can set a red threshold in the datastore properties, as suggested earlier, to prevent additional provisioning to this datastore. However, if you have thin provisioned the VM's they can continue to grow as users continue to store data on those virtual disks. if your organizations are fast provisioned and now want to persue the relocation of the VMs you can download a vmware fling called LCTREE to find out the relocate order for the VMs on the specific datastore, then use the (deprecated) relocate method to move the VMs, using the order described in LCTREE, to a less-burdended volume.
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