After unmounting NFS datastore from all hosts, <DATASTORE_NAME> (Inaccessible) is still shown in vSphere Client -> Inventory.
No host is displayed in Inventory -><DATASTORE_NAME> (Inaccessible) -> [Hosts] tab
Some virtual machines or past snapshots may be referencing ISOs located on that datastore.
Even if the virtual machine is not currently using the ISO, a reference to the datastore will remain if there is a snapshot taken while the ISO was mounted.
If virtual machines are displayed in Inventory -><DATASTORE_NAME> (Inaccessible) -> [VMs] tab, they still have references to the datastore.
To resolve this, remove the stale references. Refer the "Resolution" section in KB 345262.