No Luck, I have changed it to Ctrl + [, but still nor working.
What does CTRL+# mean, anyway?
I see the next shortcut on my list shows CTRL+SHFT+A. That I understand.
Does CTRL+# mean CTRL+SHFT+3 ?
Because, unless you have a telephone keypad, there is no single key for "#".
Either way, it doesn't work for me on LabVIEW 2012.
As you guessed in your post CTRL+# does mean CTRL + SHIFT + 3. I was also able to test this functionality in LabVIEW 2012 and this keyboard shortcut did deliver the desired functionality. It is important to note that the front panel and block diagram have separate toggles. To enable or disable grid alignment on the front panel you must have the front panel as the active window in LabVIEW. Using this shortcut with the front panel active will not affect the block diagram grid alignment.
At least in 2012: While dragging the label, press spacebar. That will stop the label from snapping to the predetermined positions.
2010 works, too.