You would need to loop, E.g.
Function CreateDictFromColumns(sheet As String, keyCol As String, valCol As String) As Dictionary
Set CreateDictFromColumns = New Dictionary
Dim rng As Range: Set rng = Sheets(sheet).Range(keyCol & ":" & valCol)
Dim i As Long
Dim lastCol As Long '// for non-adjacent ("A:ZZ")
lastCol = rng.Columns.Count
For i = 1 To rng.Rows.Count
If (rng(i, 1).Value = "") Then Exit Function
CreateDictFromColumns.Add rng(i, 1).Value, rng(i, lastCol).Value
Next
End Function
This breaks on the first empty key value cell.
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