Unregisters a folder or database from an ArcGIS Server site.
RemoveDataStoreItem (connection_file, datastore_type, connection_name)
An ArcGIS Server connection file (.ags) for the server whose database or folder is being unregistered. If you've made a connection in ArcCatalog, you can use the connection file found in your user profile directory. Alternatively, you can create a connection file from scratch using the function CreateGISServerConnectionFile.
The type of data being unregistered.
The name of the folder or database being unregistered, as it is currently registered with the ArcGIS Server site.
Unregisters a folder from ArcGIS Server that was using the alias "My local data folder".
import arcpy arcpy.RemoveDataStoreItem("GIS Servers/MyConnection.ags", "FOLDER", "My local data folder")