Yep there is a better way, DataGridViews has a property called 'SelectedRows'. So instead of you looping through every row in the DataGridView you can just use that collection:

vb.net Code:
  1. While Content.SelectedRows.Count > 0
  2.         Content.SelectedRows(0).Selected = False
  3. End While

Both your code and mine does the same, but I'm just looping through the rows that are selected and making them not selected.