I think you can't do that but atleast you can update it. In order to edit an existing row in a DataTable, you need to locate the DataRow you want to edit, and then assign the updated values to the desired columns.
Example,
DataSet1.Tables(0).Rows(4).Item(0) = "Updated Company Name"
DataSet1.Tables(0).Rows(4).Item(1) = "Seattle"