My little brother has Switch controllers that I'm going to take.
Why would you take the Swtich controllers that belong to your brother?
The reason is I want him to experience what it feels like when he doesn't get his controllers back.
It's mean to take your brother's Switch controllers. You shouldn't steal things from your siblings, as siblings are supposed to trust each other. If you steal his controllers then he's probably going to be very upset.
I want to do it because he's blaming me for something I didn't do.
That's awful that he's falsely blaming you for something, but you shouldn't take your little sibling's controllers, because then he'll have a legit thing to blame you for and you will be at fault. I think you should try to talk to him rationally and explain how his false accusations are troubling you and they're unfair.