Skye met Thor when he legitimately got lost. He knocked on her van door, delightfully oblivious to just how dangerous doing said action in New York City was. She opened the door and stared at him wide eyed.

"Hello Miss, I seem to be a little lost" she stared at him as he waved his hand across her face
"Uh miss are you okay?" Skye quickly recovered and stared at the avenger.
"Uh where do you need to go…? Mr Thor?" he then told her the address and she told which way to go, he was all set to leave when he took notice of how Skye looked. Her cheeks were puffy and her eyes were red and raw. Thor took action to remedy her upset at once.

"Madam, are you okay and do not say you are because you have been crying" she shook her head.
"You have better things to do" Thor disagreed and somehow they ended up in an abandoned park.

Skye began to pour out her heart to the Norse god without any reason to trust him.
"I don't really know why it's so upsetting I mean I hated her, she made my time at the orphanage an absolute hell it's just… I never expected her to die." Thor smiled at her warmly.
"If I may Miss Skye… this Nun is the last link to your childhood is she not?" Skye nodded
"Well… you obviously don't have a lot of people around you and since you never knew your parents I suppose it feels like you have to grow up does it not?" the realisation that spread across Skye's face made him laugh.
"I suppose… I know I didn't really like her but she still was family… I guess I get it" Thor was going to say something when a message from Natasha came through. Skye smiled sadly.
"You can go Thor… I'll be fine. Promise" The Norse god hugged her
"I hope you find a home one day Skye" and then he took off to the sky leaving a slightly happier Skye behind.