I can't do it without shipping moments, like @theresnosafeharbor4myships did, but I'm cool with that. :D Not numbered because they’re pretty random and many are probably not even things that stick out to others, but do for me.
Daryl showing up to the farmhouse with his face clean and his hair slicked back and doing the chin-tilt to Carol, and her looking at him like she did.
Carol in the church, praying for Sophia.
Glenn consulting with Dale for advice on dating in the apocalypse, and his face when Dale asked him how he knew Maggie wanted to have sex with him, and his answer about what he was thinking, having sex with her.
Dale telling Andrea "we've all wanted to shoot Daryl."
The look on Carol's face after she killed the walker Lizzie was "playing with," in “The Grove,” when she realized that Lizzie did not, after all, understand about walkers. (it's such a small thing but so beautifully done.) (Ties with Carol's face when she realized Daryl hadn't come back from Woodbury.)
The look on Merle's face in the deleted scene from "I Ain't a Judas," after Carol said she would slit his throat if he messed with Daryl, when his eyes shifted over to Daryl and then back to Carol, like he'd just twigged to how important they were to each other. (*bonus: remember the adorable little grin on Carol's face in "Consumed," when she turned away from Daryl and the painting? my head canon is that when she walked away from Merle, she had a similar little smile on her face, like "I DID IT.")
Also from a deleted scene (from "Judge, Jury, Executioner" IIRC?): "Every kind, smart thing you've ever said, take it all back, I've lost worse."
The look on Carol's face in "Consumed" when she realized Daryl had put down the walkers in the shelter for her.
Daryl telling Merle he lost his hand because "you're a simple-minded piece of shit" (tied with Daryl pointing his crossbow at Merle on the bridge to get him to leave the family they'd saved alone.)
#1: The hug to end all hugs.
ETA: Not tagging anyone, but feel free to play along at home!