You could use two ArrayLists.
For each ArrayList as an item in another ArrayList.
The "outer" ArrayList contains the rows, and the "inner" ArrayList contains the columns.
Dim arrRows As New ArrayList
For Each row As DataRow In <datatable>.Rows
Dim arrCols As New ArrayList
arrCols.Items.Add(row("first column"))
arrCols.Items.Add(row("second column"))
arrCols.Items.Add(row("third column"))
arrCols.Items.Add(row("fourth column"))
'and so on
arrRows.Items.Add(arrCols)
Next To access those rows and columns in the ArrayLists, you can do this.
For Each item As ArrayList in arrRows
variable1 = item(0)
variable2 = item(1)
variable3 = item(2)
variable4 = item(3)
Next
'Or this
someVariable1 = arrRows(0)(0) 'Retrieve the first "cell" in the first row
someVariable2 = arrRows(2)(3) 'Retrieve the fourth "cell" in the third row