I just so happened to be watching a YouTube video on that last night. The alarm will sound, which is good, but for how quick and easy it is for anyone to pop open the frunk, I would suggest against putting valuables in there as well. Within 3 seconds, someone could be running off with your laptop, tablet, hard work, etc. By the time someone would hear the alarm and look, the thief would be long on their way.
I originally thought that the frunk was the safest, most secure, place to put my valuables, because it is so isolated. But with that external manual release, it's the least safe place to put anything. The manual release should have been placed inside the passenger compartment, or a mechanical key to access the manual frunk release if left outside as it is.