Use Take and Skip to get the data rows to remove then use a for/next to remove the rows. Here I delete the first three rows.
Dim table As New DataTable()
table.Columns.Add("SomeColumn", GetType(Integer))
For index As Integer = 0 To 9
table.Rows.Add(index)
Next
Console.WriteLine(table.Rows.Count)
Dim rows = table.AsEnumerable().Take(3)
For index As Integer = 0 To rows.Count() - 1
rows(index).Delete()
Next
Console.WriteLine(table.Rows.Count)