A.S.
Can you firmly (and repeatedly, of course,) let him know that he cannot go anywhere in the car unless he remains fastened in his seat? Also, if you are wearing headphones, he probably is mad that you are tuning him out. Have you tried listening to some kids' music in the car? Baby Beluga by Raffi, for example, is soothing music to my ears. Maybe try classical music, as well. Whatever you do, this will last until he understands that you WILL keep him in his carseat. Also, eventually he should get tired of being so upset. I feel for you.
Amy