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I'm working on my first kit guitar (stew mac triple-o) and have glued the sides to the neck block and tail block. Now that the clamps are off, I can tell that the neck block is severely misaligned. It's centered properly at the back of the guitar, but is visibly off-center at the front.

Is it possible to unglue the neck block in order to get a second shot at alignment (it was glued with Titebond)? Or is my only option to start over with new sides and blocks?

Taking off the block is not impossible , Get a cloths iron set to med heat. You also need a very flexible knife. Set the iron on the area when the neck block is glued. Let set about 2 minutes and see if the knife will work into the glue joint. Don't force it , you will feel the glue loosening.
As soon as the glues starts to release keep working the knife in the joint. Once you have it separated , clean off the old glue. You also want to set the neck into the neck block and check the neck center to the neck blocks center. Never assume the neck mortise is centered to the neck block. Use the neck center as the neck block center if there is a difference.
Once you establish the center make a mark on the back part of the neck block. Tape the side set together Dry fit the neck and apply tape from the outside of the rim over the top so the neck block is hinged to the side set. Apply glue and be careful regluing as glue is a lubricant when it is wet. Clamp Check adjust , clamp and get it right.

Hehe Rick you were typing faster than me

Yeah, it's possible! I had to Reglue the tail block because the clamps slipped. I used a hair dryer and a putty knife I thinned down on my belt sander. Keep the heat moving though and don't force the knife. Let the heat do the work and soften the glue. An iron might have been Better though.

Taping the side set together is a great tip John. Wish I had done that.

and don't forget the de-glue goo to clean up the glue residue once it's apart. You don't want any residue left when you go to reglue it.

While we're on this topic of ungluing, how does one unglue a fingerboard from the neck? It's detached from the body.

I use a heat blanket but a cloths iron will work , It is the same principal , heat and a flexible knife. Let the heat do the work , should be off in 15 minutes or less .
I start at the heel , let the iron on Med heat , allow 2 minutes then start checking to see if the heat is getting through the wood. Once the glue heats to about 160 degrees it will soften . You need to be firm but don't FORCE.

Do I have to remove the frets first?? I intend to eventually.

you can do it either way

I use this knife along with a fretboard heat blanket and usually start from the other end. In this instance I was repairing truss rod so I had cut through the 1st fret and only took off that part. The knife provides a nice wedge action that lifts and doesn't cut into the wood.