After the women's free skate, Canada was already locked in first place, with ice dancers Tessa Virtue and Scott Moir still left to compete.
With the pressure taken off them, the duo blew away competition, finishing first with 118.10 points, six points ahead of Americans Maia and Alex Shibutani, who helped their country win bronze.
The Olympic Athletes from Russia, with a stunning free skate by 15-year-old Alina Zagitova, the European champion, were guaranteed silver, the team's second medal of the Pyeongchang Games.
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The 27-year-old Chan, who had struggled with his jumps in the team event's short programme, landed the first two quads of his free skate, earning him a season's best score of 179.75 points.
Skating in his third and final Olympics, Chan was inconsistent on his other jumps, rushing on his takeoffs and doubling a triple Axel before falling on the next one.
"I'm just happy I did the best I could and I left nothing, no rock unturned," said Chan, who admitted his nerves were jangling and he "just had a conversation with myself" to get back on track.
"I achieved a big thing, which was to land the two big quads in one programme. I'm going to hold this medal tight to me and it's going to be as good as the individual event."
Chan, who won silver in the team and men's singles events at the 2014 Sochi Games, is a three-time world champion but Olympic gold had evaded him until now.
Daleman, who won bronze at last year's world championships, landed a series of triple jumps in a stellar performance that saw her finish third, only 0.39 points behind second-place finisher Mirai Nagasu of the United States.
Zagitova, skating at her first Olympics, turned in a sizzling performance to composer Leon Minkus's "Don Quixote."
Skating in a flashy red tutu, the 15-year-old scored 158.08 for a season's best to take first place.
Nagasu became the first American woman to land a triple Axel at the Olympics, cleanly hitting the jump at the start of her programme to gain a season's best score of 137.53.
Clearly overjoyed, the 24-year-old - who wept after being left off the Olympic team for Sochi in 2014 - pumped her fists and grinned as she skated off the ice.
Asked about the fact that she is only the third woman to land a triple Axel in the Olympics - after Japan's Midori Ito and Mao Asada - Nagasu, the daughter of Japanese immigrants who run a sushi restaurant, joked that maybe it was her ancestry that helped.
"I feel really great. Going into it, I was like a train, get on those tracks and get some speed," she said. "To nail it the way I did - and even out of the corner of my eye, I could see my team mates standing in excitement."
"Maybe it's the Japanese genetics - but lucky for me I'm American, so I'll be the first U.S. lady."