一旦、Dictionary に変換してやってみました。
( 二次元配列ではなく、ジャグ配列になってしまいますが。)
Private Sub Button1_Click(ByVal sender As System.Object, ByVal e As System.EventArgs) Handles Button1.Click
Dim a1 As String(,) = {{"SN01", "aa1", "bb1"}, {"SN02", "aa2", "bb2"}}
Dim a2 As String(,) = {{"SN01", "cc1", "dd1"}, {"SN02", "cc2", "dd2"}}
Dim dict As New Dictionary(Of String, List(Of String))
AddToDict(dict, a1)
AddToDict(dict, a2)
Dim lst1 As New List(Of String())
For Each kv As KeyValuePair(Of String, List(Of String)) In dict
Dim lst2 As New List(Of String)
lst2.Add(kv.Key)
lst2.AddRange(kv.Value)
lst1.Add(lst2.ToArray())
Next
Dim a3 As String()() = lst1.ToArray()
End Sub
Private Sub AddToDict(ByVal dict As Dictionary(Of String, List(Of String)), ByVal a As String(,))
For i As Integer = 0 To a.GetLength(0) - 1
Dim lst As List(Of String)
If dict.ContainsKey(a(i, 0)) Then
lst = dict.Item(a(i, 0))
Else
lst = New List(Of String)
dict.Add(a(i, 0), lst)
End If
For j As Integer = 1 To a.GetLength(1) - 1
lst.Add(a(i, j))
Next
Next
End Sub
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