I'm getting to the point of frusteration with the new crossbows. They do not fire in the same way a bow and arrow does and it is making me miss my shots time and time again. Tips for ranged combat with these things?

Practice. They are not bows so you have to practice. PRACTICE!!!

Press and hold down the trigger while you aim. For what it's worth, the bolt isn't dead on for some long shots as it goes a little bit up and to the right. So compensating for that I was pulling off head shots in no time. Just aim a little down and to the left, think I would aim for the shoulder (right) and it would smack them in the head.
Truthfully, I found the crossbows to me more accurate than bows. But thats me

I always test new bows on the targets in any town. I did for crossbows, too. Go test different ranges and get to know how they work.

FYI, I do this even for different types of bows as some can even be different from type to type.