I don't think so, I'm fairly sure that would get all the fields in one datarow (ItemArray is another way of referring to fields in a datarow, just in the form of an Array instead of .Item("Name")).

I don't think you want to do this directly from the datagrid, as the datagrid is just a mouthpiece for a datasource (unless of course you're typing in rows at runtime) - you may want to query the datasource and then work with the data it contains. May I ask why you want to turn the contents into an array? You may not really need to, you can for example:

Dim iCount as Integer

For iCount = 0 to (dsData.Tables("Table").Rows.Count - 1)
DoSomeFunction(dsData.Tables("Table").Rows(iCount).Items("Column"))
Next