You know, a do loop would work just as well as a goto. People might make fun of you if you use gotos.
Look at where your end select is. (wink wink).
Not that your way is wrong, but another way to do what you're doing is to use an array, such as
dim dienumbers(5) as integer
then, you could do
DieNumber = CInt(Int((6 * Rnd()) + 1))
other stuff
dienumbers(dienumber-1) = dienumbers(dienumber-1) + 1
other stuff
Freq1.items.add(dienumbers(dienumber-1))
Since the array starts at 0, all values for one would be stored in dienumbers(0), and all from 6 would be in dienumbers(5). If you didn't mind, you could waste the first element of the array and use dim dienumbers(6) and dienumbers(dienumber) = blah.
The benefit of this way is not as much typing for you
This is the first time I've seen vb.net code. Doesn't look too different from vb6. What is with the ") Handles Calculate.Click"? Can you specify the subroutine for an event?