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Demons weren’t supposed to be able to love. It was a defining feature. Demons couldn’t love, just as angels had to love. Once an angel Falls, they’re incapable of sensing the love others exude. Crowley knew this, and yet he still felt love. Felt loved.
Angels were, technically, not able to fall in love. They loved all of God’s creations, of course, but that was an all-encompassing thing. Falling in love was a form of favoring one creation. It wasn’t allowed. Aziraphale knew this.
And yet he sensed such intense love from Crowley in the Garden. He had assumed it was just love for Earth, or for Eve and Adam - Aziraphale had seen the demon occasionally help the two in the Garden, taking care of Eve when she was expecting and Adam was wandering. This was further solidified by Crowley helping the two take care of their children. And after that it was easy to brush the growing love in the world off, chalking it up to the growing population.
Crowley never sensed any fear from Aziraphale - well, not towards him, anyway. Some exasperation, but the edges of the feeling were soft. Crowley interpreted it as fond.
Aziraphale realized he had deviated even further by falling in love with Crowley in 1793. When the demon saved him from execution. He discovered, after some thought, that he had probably fallen in love sometime before Rome. He knew nothing could come of it - demons couldn’t love, not to mention his duties to Heaven.
Crowley knew he was in love with Aziraphale after the incident with Job. The angel had lied to help the children even believing he’d Fall for it. Crowley felt such a deep rooted affection for the other that he knew it couldn’t be anything else. He hated it, thought it was stupid, that it would break his heart one day.
They blamed the humans.