Hi @EvanBlank ,
If the datastores are provided from local disks, check the server management console for hardware errors and volume management.
In case they are NFS or iSCSI you will have vmkernels assigned to them, check for network connectivity to and from these vmkernel's IP Addresses.
I would also check what is the status of the volumes in the storage management interface. Assuming this is an EMC Unity (from the datastores name description), this interface is the Unity Unisphere, which can be accessible via browser. From there you will be able to check the status of your volumes and disks and if/how they are interacting with your vCenter/ESXi hosts.
You will also be able to mount/unmount the volumes from there, as suggested.
Best,
