In the world of The Smurfs, Gargamel the Evil Wizard is the sworn enemy of the Smurfs and always tries to capture them. He is the main antagonist in the show and comic books. His main goal in life is to destroy the Smurfs or to capture enough of them to create a potion to turn base matter into gold.

He is the main antagonist who, along with his cat Azrael, and later with a young apprentice named Scruple, continued to plot against the Smurfs in order to capture and/or destroy them. He was responsible for the creation of Smurfette, who was changed into a real Smurf by Papa Smurf. Gargamel is a hateful individual who is willing to commit many sinister and cruel acts to achieve his goals and he can be downright ruthless on occasion, such as enjoying tormenting the Smurfs, threatening to burn Puppy alive, and even attempt to harm the defenseless Baby Smurf. He has even gone out of his way to simply make sure to ruin the happiness of others. However, despite his dark and evil heart, there have been a few occasions where Gargamel has shown a small amount of genuine emotion, most notably with Azrael, who Gargamel has shown real care for on rare occasions despite mistreating him and even goes against Lord Balthazar to defend his cat, claiming that Azrael is all he really has and is quite possibly his only real friend. Also, when he was once forced by Balthazar to behead Puppy with a guillotine, he pleaded with his godfather to find another way before submitting to Balthazar's intimidation.

Gargamel's cruelty and evil nature seems to stem from a harsh life and upbringing. One example being that Gargamel hates having his Birthday on Halloween because every year nobody wishes him a Happy Birthday or gives him a present, and all Gargamel really wants is for somebody to remember his Birthday. His mother often mistreats him and tries to make him more evil, while also resenting him for flunking Wizard's School. Deep down Gargamel is lonely and insecure due to being ugly and even admits that no one has ever genuinely said they loved him. In the cartoon show episode "They're Smurfing Our Song", Gargamel is revealed to indeed posses a small amount of goodness somewhere in his heart, as shown when he was moved to tears by Sassette's kind and loving words as even the force of evil within him could not withstand Sassette's love as she was the first person to ever say they loved him. When affected by Woody's magic pan flute, Gargamel's inner goodness was brought out due to finally feeling happiness after so long and he revealed to Papa Smurf that he had not been his true self in a long time due to his many years of hate and even apologized to him, and Papa Smurf accepted his apology, knowing full well that everyone had good in their hearts somewhere. The spell of happiness that brought out his goodness was only temporary, but according to Papa Smurf the memory of the event would remain with Gargamel forever.