A more specific favorite would be in Season 2, when Rumple makes that phone call to Belle after he was stabbed by Hook. It was so sweet and honest, and I think that is the Rumple that we need to see in order for him to be redeemed.
A very very very close second would be the Rumbelle phone call followed by the Nealfire/Rumple moment of holding hands.
I have to go cry now
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"He was a lot of things to me" "The only conclusion was love"