How can I increase my crush's comfort when I'm around her?

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You stated three completely separate things that you think all go together but they don’t.

That you need to increase her comfort.
That you’re a high value guy.
That she doesn’t see you as boyfriend material.

None of these things matter for any of the others. If you’re a “high value guy” that won’t make her want to be your girlfriend or make her comfortable around you. If you make her more comfortable around you that won’t get her to see you as a high value guy or want you to be her boyfriend. If you were her boyfriend, that wouldn’t make you a high value guy, and wouldn’t necessarily mean she’s comfortable around you, though women typically select for comfort in boyfriends, especially as they get older, they don’t all the time. Sometimes they like bad boys that keep them on their toes.

If she is attracted to you and you are attracted to her, there’s only one thing really to do, and that is connect physically. Relationships happen after a physical connection is made, not before. You can talk all day long, you can look at each other all day long, but unless you’re comfortable touching each other than you will never have a relationship with her.

Some things to do:

Touch her lightly on the arm when you are talking to her whenever you make a point and you want to emphasize it
Hug her when you first meet and before you leave each other
Hold hands
Put your arm around her when you are spending time together
Go for a kiss, but don’t get discouraged if she turns you down. Keep trying, but not more than once a day.
Massage her back. Get daring and venture down to the upper buttocks

Once you’ve had a first kiss, amp up the physical contact.

Hug her from behind when she’s not expecting it.
Caress her face
Massage her butt and legs
Nibble on her neck
When you are holding her, cup one of her breasts. Resist the temptation to knead, just hold it. If nobody is looking, you can try to slip it inside her shirt.

Holding hands seems to be the thing to shoot for when you are dating, if you do that regularly then you can move up to kissing. If you’re regularly making out then that qualifies as a relationship in my book and it’s only a matter of time before you have sex.

You don’t want to move too fast through the steps, but don’t dilly-dally either. If you’ve kissed and it’s been a month and you still haven’t had sex, you should move on. Work on more physical contact with the next girl.