Wearing a red tutu, the 15-year-old demonstrated her ability to bounce back after a rough short program on Friday in which she fell on her triple lutz triple toe combination, as well as on her triple flip.
"The competition isn't done yet", the Spaniard said.
Japan's world silver medalist Shoma Uno is now second but crashed on his quadruple flip and has 93.92 points. "I didn't think I would be able to execute my jumps".
Osmond, the world silver medallist who won the Skate Canada event last month, failed to capitalise on her lead in the short programme, finishing third with 206.77 points.
An energetic performance by France's Vanessa James and Morgan Cipres saw them take second place, finishing almost five points behind the Russian pair.
However, Maria Sotskova and Alina Zagitova of Russian Federation passed the Canadian to claim silver and gold with scores of 140.99 and 151.34, respectively, on Saturday.
"Jeu du piment" : la gendarmerie alerte sur un nouveau jeu dangereux
Jeu du foulard , ice and salt challenge, jeu de la tomate ou jeu de l'escalier . Ce nouveau "jeu" consiste à rapporter des piments à l'école.
Double world champions Gabriella Papadakis and Guillaume Cizeron impressed in front of their own fans in the ice dance, and lead the way on 81.40 points.
Performing to Ed Sheeran, the French couple produced strong footwork and a straight line lift and bagged a personal best.
Americans Madison Chock and Evan Bates are their nearest challengers on 73.55 with Russia's Alexandra Stepanova and Ivan Bukin third on 70.02.
Russia's Evgenia Tarasova and Vladimir Morozov, the bronze medalists at this year's world championships, finished first in the pairs with 77.84 despite being out of sync in the step sequence at the end of their short program.
A big triple twist was the highlight of their routine and pushed home skaters Vanessa James and Morgan Cipres into second on 73.18.
The men's and women's free programs will be held on Saturday.
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