Hmm. This seems like an odd request.
Databinding directly to your datasource is going to be out of the question since, as you probably know, you can only bind to 2 columns within a DataSource. (DataTextField and DataValueField)
What you are probably going to have to do is some logic such as this
For Each dr As DataRow in dt.Rows
For Each dc as DataColumn in dt.Columns
dropDownList1.Items.Add(new ListItem(Convert.ToString(dr[dc]), Convert.ToString(dr[dc])))
This code will iterate through each Row in your data source and then iterate through each column in each row of the datasource (here i have assumed that dt is of type DataTable). Is this what you are looking for?
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