Shoma Uno of Japan was second with 100.28 points after landing all his jumps cleanly, while Olympic champion Yuzuru Hanyu had 97.04 in third.
"I'm very happy with the way things went," Chen added. "There were a few bobbles here and there, like in the ending position of the program. I think that one was a little funny actually, but it's something that I'll work on for worlds."
Hanyu opened with a quad loop, but could only manage a double salchow instead of a planned quad salchow as part of a combination jump that included a triple toe loop.
Jin Boyang of China was fourth with 91.33 points
Patrick Chan of Canada fell on his opening quad toe loop and stumbled on the landing of a triple toe loop to finish in fifth place with 88.46 points.
Virtue and Moir, first after the short dance, scored 117.20 points in the free dance for an accumulated 196.95 points overall to capture their third Four Continents title.
"Today was an interesting performance for us as we left a couple of points on the board, but it was really special for us to be in that venue," Moir said of the 2018 Olympics site. "We really felt the energy and we're really happy with certain parts of our performance. We're going to be pretty excited, looking forward to the next five weeks for the world championship."
Maia Shibutani and Alex Shibutani of the Unites States earned the silver medal with 191.85 points, and teammates Madison Chock and Evan Bates claimed bronze with 185.58.
The Shibutanis fell during warmups.
"The warmup today was a little bit unusual," he said. "We both went down on a very simple thing. I think that we're both very tough competitors and very mentally strong, so it didn't bother us. We took the time to do what we needed to do and we focused on executing the performance we were planning on. We're very proud of how we handled it."
The women's and pairs free skate is on Saturday.