Every scene with Cal on the witness stand being cross-examined by his ex-wife.
In "React to Contact", Cal and Emily exit an office where the client of the week's son Jake is playing. Cal does a quick introduction as they walk, while Jake immediately starts chatting up Emily. Cal verbally chases her down the hall, and once she's gone, stares at Jake for a long moment (apparently he read something he didn't like). He's like''nine''. But then, Emily with her school uniform...can't blame the kid.
Emily studying for and taking her driver's test in "Delinquent", mainly for Cal screwing with her by screaming "PUPPY!" (causing her to crash into a fire hydrant) and their banter at the end.
Reynolds and Lightman betting on what the photographer would say when they found the gay porn they knew he was into:
Cal: 'It's for research' I win, 'it's not mine', he wins. Thanks, mate.
Made even better by a scene earlier in the season where Emily calls him out on a photo of his younger self with a tribe he was studying, clearly baked, to which he immediately responds "It was research." She doesn't buy it, either.
Cal talking to the shrink at the mental institution, pretending he's delusional and hears voices . . . and oh yes, Reynolds is trying to make him kill people. First, we think it's just Cal fucking with authority figures, then we realize he's trying to get himself committed.
Crosses the Line Twice when Cal gets the info he needs, tries and fails to convince the shrink he's not mentally-ill, walks out of the ward . . . and is immediately picked up by two orderlies and carried back in.
Cal: Worth a try.
YMMV, depending on how dark your humor is, but "YOU OWE ME TWO-HUNDRED BUCKS YOU BASTARD" also can be counted as a Crowning Moment of Awesome.
Drunk!Gillian and Torres in "The Canary's Song", especially Gillian's "up yours!" toast to Cal.
Cal asking the undercover federal agent how he manages to keep his eyes open after being "shot to death" with blanks.
The attempted intervention at the end of "Greivous Bodily Harm".
This exchange between Emily and Cal might just be the funniest thing I've ever heard
Emily: Dad!Don't use any kind of psychological tricks to scare my boyfriend!
Cal: No Tricks! Got it! (opens door for Emily's Boyfriend)