As with all Robot Chicken episodes, the stories use rather adult humor and are not considered suitable for general audiences. They are also considered "non-canonical" Smurf stories.
In one story "Murder In Smurf Town X", the Smurfs investigate the deaths of seven fellow Smurfs, in a parody of the thriller movie Se7en. Baker's death represents gluttony, Vanity's death represents pride, Lazy's death represents sloth, and Chronic-Masturbator Smurf (a non-existent character) represents lust; however envy, greed, and wrath were never shown, but likely Greedy was among the victims and that goes with Grouchy who represents wrath. In the end, Brainy, in charge of the investigation, finds out the culprit is Jokey, who decapitated Smurfette and gave her head to Brainy before it explodes. The story ends with Papa Smurf dancing with Smurfette's headless body with an acorn for a head and her hair taped on it.
In another story "Smurf-tastrophe!", Anderson Cooper investigates the flooding of the Smurf Forest, after Papa ignores Army Corps of Engineers Smurf (a non-existent character) and his warning about the dam. Several dead Smurfs float by Gargamel's door, who gladly scoops them up to eat. However, he finds that the Smurfs don't taste good after all, and orders Chinese instead.
In a third story "Tastes Like Rotten Smurfberries", the Smurfs and the Snorks are at war with each other over sewage-related water pollution, but make peace after the discovery of the Snorks' multiple females.
In a fourth story "Smurfatar" (a parody of the James Cameron film Avatar), Gargamel transfers his mind into a Smurf body and infiltrates the Smurf Village as "Gargle Smurf" to destroy them. However, he comes to see that Smurf life is good after all.
In a fifth story "Not So Smurfy" (a parody of The Hunger Games), the Smurfs' village faces infestation by gypsy moths, which eat all of their smurfberry crops; with the Smurfs facing starvation, Gargamel capitalizes it by hosting a tournament, in which all of the Smurfs fight to the death for a prize of Gargamel's smurfberry crops. The Smurfs are freed when Azrael eats gunpowder and Gargamel kicks him while ranting about his lack of sexual gratification. Sassette Smurfling (voiced by Kesha) then proceeds to kill Papa after he ignores her suggestions on how to avoid another famine, going as far as to cut his beard off and wear it, all while shouting "Who's your papa?!" and forcing the other Smurfs to bow to her.
In a sixth story "Undercover Smurf Boss" (a parody of Undercover Boss), Papa Smurf goes undercover to see how his village really runs. He finds out that the Smurfs have been living off of caterpillar milk this entire time. Also, Farmer Smurf's hands have gotten so bad that he's had his wrists locked in place because health care costs are so high. When Papa heads to the doctor's office, Doctor Smurf leaves him in charge and dips out in a gold plated helicopter. Handy Smurf comes in missing all of his fingers, and it's up to Papa Smurf to fix it. Later, he encounters Grouchy Smurf who proceeds to tell him all of the things he hates. This leads Papa to have him shovel dog poop after he's done with the show.
In a seventh story "House of Smurfs" (a parody of House of Cards), the village holds an election to be Papa Smurf's second-in-command. Brainy assumes it will be him; instead, he once again gets thrown onto his head. The constant head trauma has given him a lack of moral compass and a Southern accent. Brainy conducts an unscrupulous campaign that includes teaming up with Gargamel, blackmailing Handy Smurf, and getting political favors by seducing Smurfette. Hefty Smurf ends up winning the election and as soon as he does, Gargamel attacks and kills Papa Smurf with a mallet. Brainy is there for the rescue with a gatling gun that Handy built for him. Smurfette calls for another vote and Hefty wins again on sheer looks alone.
In an eighth story "Smurf Memorial Day", the Smurfs celebrate Memorial Day. Papa Smurf names some dead Smurfs, such as Myspace Smurf, Payphone Smurf, Talk to the Hand Smurf and Michael Dukakis Smurf, who Handy Smurf notes are outdated. Curious, Handy wonders if they all died of natural causes. A flashback shows all the Smurfs who outlived their usefulness being killed via gunshots. Papa shrugs that those were natural deaths, but Handy is suspicious. Papa later meets with Azrael, paying him to assassinate Handy for getting too close to the truth.
In a ninth story "Suda-Smurf", Brainy (on top of Handy, Jokey, and Hefty hidden within a trenchcoat) attempts to buy boxes of Sudafed from a pharmacy in order to make Crystal Meth. The pharmacist at the counter says they don't serve Smurfs, Brainy then trying to fool him into thinking he's not obviously a Smurf. When that fails, Brainy gives him a gift box from Jokey, which explodes and allows the Smurfs to steal the drug and leave. The segment then ends with mugshots of Brainy and two others on Meth after being arrested.
In a tenth story "Brainy Smurf Gets CTE", Brainy tells Smurfette he can't find his glasses when they're right on his face. This leads to Doctor Smurf diagnosing him with Chronic Traumatic Encephalopathy as a result of him being tossed on his head too many times. Doctor says treatments aren't very effective and gives Brainy a loaded handgun, which he immediately shoots himself with. Papa Smurf is enraged by this, Doctor then revealing that he is actually Costume Party Smurf (a non-existent character).
- Danny Goldman reprises his role as the voice of Brainy for the first four stories.