Aw Kat, I can only imagine that this all must be so incredibly stressful and overwhelming for you to try to think and wade through, about what may or may not be truly helpful for your sis right now.
I tend to agree too with everyone... maybe your sweetie and stepdad and two of their good friends, could just 'happen' to stop by on their way to somewhere and visit the boyfriend to 'offer their help' in assisting him to leave the country. Since your sister herself gave this as the reason for his visit that day, it is simply an offer to help him. If they happen to look intimidating and involved, well, it's not their fault they are big guys, right?
The odd phone call and overheard arguing by your niece's friend - keep this in mind. No matter how much he loves her, clearly he is a genuinely and extremely ill man in need of professional treatment; there is no escaping the fact that his influence and presence in her life is a danger. He is not bringing out the best in her certainly and she needs to face the fact that, as much as she might like to, she is simply NOT strong enough to act as his saviour.
I really know nothing about interventions but I am sure one of these crisis counselling places could help provide you with some professional information and guidance. I appreciate that your family does not want to do the wrong thing or take a wrong step right now...

but I would not rule this out too quickly if this was recommended.
Oh, and I would copy your letters to the Chief of Staff of any hospital that was involved in his release!
Kat my thoughts are with you.
Love and hugs!
mig