As a more proper and sure way, I would get each picture box, keep handles and locations of them, then sort them according to their location. Now they are ready to use. Here is an example:
Public Class Form1
Structure Pbox
Dim handle As IntPtr
Dim top As Integer
Dim left As Integer
End Structure
Dim pboxlist As New List(Of Pbox)
Sub ClearImages()
pboxlist.Clear()
For Each c As Control In Me.Controls
If TypeName(c) = "PictureBox" Then
Dim x As New Pbox
x.top = c.Top
x.left = c.Left
x.handle = c.Handle
End If
Next
pboxlist.OrderByDescending(Function(a) a.top).ThenByDescending(Function(a) a.left)
For Each item In pboxlist
Dim x As PictureBox = PictureBox.FromHandle(item.handle)
x.Image = Nothing
Next
End Sub
End Class
Another approach is using a good naming, so that you can use their names to sort them. For instance, PictureBox1 will come before PictureBox2 if you sort. So you should use PictureBox1 for the very top and left one and PictureBox2 for the next one and so on...
EDIT: Using Tag property, as John Bustos suggested, instead of names is an easier and better idea. So without getting lost in names, you can sort picture boxes according to their Tags which are defined by you.