Personally, I can't pick just one episode with the best Callian moments. From season one it's Pilot (01x01) of course, Blinded (01x12) and Sacrifice (01x13).
Season 2: Honey (02x04), Black Friday (02x07), Secret Santa (02x08).
But if I would have to pick, I'd pick Honey, for the end of the epi. :)
I cant chose just one, but Honey is definetly one of my favourites because of when Gillian loses it when Cal getts taken hostage and when hes at her doorstep at the very end.
Honey, of course, but also Darkness and Light for one of the best openings EVER <3 and now, inevitably, The Canary's Song :D
And honestly, there are so many others-- small little moments that I will always remember with flailing :) Hopefully, we'll get even more soon.