The film opens with Papa Smurf (Mandy Patinkin) introducing all the Smurfs in the village - Clumsy (Jack McBrayer), Hefty (Joe Manganiello), Brainy (Danny Pudi), Grouchy (Jake Johnson), Baker (Gordon Ramsay), Vanity (Titus Burgess), Jokey (Gabriel Iglesias), plus Nosy, Paranoid, and Table-Eating Smurf, among others. Then there is Smurfette (Demi Lovato), who was created by the evil wizard Gargamel (Rainn Wilson) from a lump of clay to go into the Smurfs' village and steal their magic. Papa used his own magic to make Smurfette good like the rest of them, but nobody is quite sure how to explain just what Smurfette is.
Smurfette is invited by Hefty, Brainy, and Clumsy to go Smurf-boarding with them. Meanwhile, Gargamel is continuing to do what he can to get his hands on the Smurfs. He sends his pet vulture Monty to go down and get some Smurfs. After Smurfette goes up for boarding, she lands in a spot where she sees a pair of eyes. She follows the creature until it sneaks back through a crack in a wall separating the Smurf village from the Forbidden Forest. She sees that the creature dropped a hat similar to her own, only made from a different material. Smurfette's friends find her but she is suddenly snatched by Monty as he flies back to Gargamel's lair.
Gargamel throws Smurfette into a cage as he snatches the hat away from her. After throwing part of it into his cauldron, he and his cat Azrael discover that the hat came from another village of Smurfs beyond the Forbidden Forest, with his only clue being an image that looks like three trees. While Gargamel is distracted, Hefty, Brainy, and Clumsy make it inside and break Smurfette out. Gargamel spots them and tries to capture them, but the four escape. When they get back to their village, they are discovered by Papa, who is not happy that the Smurfs went past the wall. He grounds them as punishment.
Smurfette sneaks out that night to go through the wall. Hefty, Brainy, and Clumsy all follow and join her. Once they make it through the other side, they are grabbed by live flowers that try to eat them. The Smurfs break free from them and soon run into flying creatures that breathe fire, which Brainy decides to refer to as dragonflies. Gargamel then shows up with Azrael and Monty. He causes Clumsy to grab one of the dragonfly eggs, leading to the other dragonflies to chase after the Smurfs. The Smurfs fall into holes while the dragonflies breathe fire down there, making Gargamel think they are dead.
The Smurfs are now separated in the tunnels. Clumsy grabs an explosive liquid that Brainy invented and uses it to blow a hole in the wall. They are found by glowing bunnies. Smurfette gets one that she names Bucky and uses him to lead her and her friends out of the tunnels. Bucky takes them by a floating river, leaving the Smurfs to ride it out themselves since Bucky knows it's dangerous. On the river, they run into Gargamel again. When he tries to attack, the Smurfs knock him and his pets into the water. Gargamel then flails around crying for help, so Hefty feels guilty and gets his friends to go back to help them. Predictably, Gargamel returns the favor by knocking the Smurfs off their raft and taking it from them.
Back in the Smurf village, Papa goes to talk to Smurfette. When he doesn't get a response, he goes into her house and sees she's not there. He goes to the homes of Hefty, Brainy, and Clumsy to find that they snuck out as well. Papa is not happy.
The Smurfs end up in Smurfy Grove, the lost village of Smurfs. They are found by a whole other group of Smurfs, all of whom are female. They meet SmurfLily (Ariel Winter), the Smurf that Smurfette saw earlier. Then they meet the hyperactive SmurfBlossom (Ellie Kemper), tough and suspicious SmurfStorm (Michelle Rodriguez), plus the many other Smurfs, along with their leader, SmurfWillow (Julia Roberts). Smurfette warns the villagers about Gargamel and his impending arrival. When Smurfette shows them the three trees, Willow says they were looking at it upside down and are looking at waterfalls, seen just past the lake. Storm says that if Gargamel saw trees, then he would end up in the Swamp of No Return (which he did). Storm goes out on her dragonfly with Clumsy to keep an eye out on Gargamel or other unwelcome intruders.
Clumsy and Storm ride high above the clouds and are spotted by Gargamel once he gets out of the swamp. He sends Monty to go after them. Storm fires her arrows while Clumsy steers the dragonfly. He then lights an arrow on fire and gives it to Storm so she can hit Monty. He goes flying down and lands in Gargamel's arms.
Upon returning to Smurfy Grove, the others find that Papa has made it by riding a glow-bunny. When the other Smurfs learn that Smurfette was created by Gargamel, Storm accuses her of being there to capture them for his schemes. Gargamel then emerges and starts using his freeze balls to capture all the Smurfs he can grab. They don't work on Smurfette because she's not a natural-born Smurf and she just absorbs the energy. Gargamel taunts her and thanks her for leading him to them. He leaves Smurfette alone crying. The forest creatures gather around her to comfort her. Brainy's pet ladybug (who also acts like a camera) comes around to remind Smurfette of her friends. She then hatches an idea.
In his castle, Gargamel starts to use Clumsy and some of the other Smurfs for his machine. He begins to take in their magic until Smurfette walks in. She pretends to be in league with Gargamel and asks that he distribute some power to her. He does so, but she just absorbs the magic and uses it to release her friends and to shoot Gargamel, Azrael, and Monty out of the castle and back to the Swamp of No Return where they are chased by piranhas. The Smurfs are free, but Smurfette's act has caused her to revert back to clay. The Smurfs sadly take her back to the village.
All the Smurfs from both villages come together to mourn Smurfette. They lay her down in a bed of flowers and hold hands. Together, their love produces magic that revives Smurfette. Her friends embrace her and they all get together for a celebration. The Smurfs then decide that Smurfette is whoever or whatever she wants to be, and they love her for it.
*CUT TO THE CHASE*
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Smurfette wants to find her place and purpose within her village. She encounters another Smurf from a previously unknown village hidden past the Forbidden Forest. With the help of Hefty, Brainy, and Clumsy, she ventures out to find the other Smurfs before Gargamel can and use their magic for his evil deeds.
The Smurfs find Smurfy Grove, home to a group of female Smurfs. Gargamel ends up finding and capturing them. He begins to absorb their magic for himself until Smurfette goes to his castle to save her friends. Because she can absorb Gargamel's magic instead of being affected by it, she uses the magic against him to defeat him and save her friends, but it causes her to turn back into the clay she was made from.
Both groups of Smurfs bring Smurfette back to her home village to mourn her, but their love for her is enough to create a magic that brings her back to life. All the Smurfs then celebrate and begin to live as one large group.
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