I think you need to use row.Delete()
http://msdn.microsoft.com/en-us/library/system.data.datarow.delete[
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I don't know if you are using a data adapter to update the source database table or not, but thought I'd add this.
Removing the row from the dataset's datatable will not remove the data from the original source database table, however using the delete method will mark it for deletion, so if you use dataadapter.update(dataset) it will delete the rows from database table that are marked for deletion.