We might as well start off with the time that the most troubling elements of the Smurfiverse collided into one hugely smurfed-up mess: "Heavenly Smurfs," the second season episode in which the Smurfs terrorize Gargamel with the threat of eternal damnation in a lake of fire.
Okay, admittedly, they have a good reason for it, and it's not like they were entirely unprovoked. Gargamel, as you might recall from babytimes, was a pretty bad guy whose lack of morals was only matched by his lack of fashion sense. In "Heavenly Smurfs," Gargamel's out trying to do some murders when he winds up knocking himself out, and the Smurfs decide to take advantage of the situation by convincing Gargamel that he died and had been sent to the afterlife.
At first, as the name implies, they use a fog machine and a set of harps to create the illusion of heaven, but quickly reveal that Gargamel's life of sin and depravity has earned him an eternity being tortured by Satan, who is here represented by Hefty Smurf with a pitchfork. Much like Ebenezer Scrooge, he is offered the chance to reverse his fate if he changes his ways, and at first, this seems like a pretty good deal all around. People have changed their ways for worse reasons, after all, and if Gargamel actually becomes Goodgamel, the ends would justify a little blasphemous gaslighting, right?
Unfortunately, as ever, the nature of man and Smurf tends towards cruelty. As Gargamel attempts to be a better person, the Smurfs decide to take advantage of this by ordering him to perform manual labor around the village. In other words, they were gaslighting Gargamel into slavery with the threat of Hell. That doesn't seem very Smurfy, now does it?