You do not control your players and cannot make them do things they do not enjoy
This is a cardinal rule of DMing. You are not the only person at the gaming table. If your players do not want to play a particular way, you cannot force them to (at least, not for very long, before they quit).
You thought that what you saw a player do in Critical Role was cool, and are wondering how to get your players to do that for you. You can't. The best you can do is get them to watch the same Critical Role episode and hope that they have the same reaction you do, and decide to want to do it for themselves.
That said, mechanically, there are two ways to handle magical mind control, and you should prefer the one that fits your players better.
Option 1: Use your powers of description to help them get into character while mind controlled.
This works well for players that already want to roleplay partial mind control, or who are at least willing to try it.
Most players are not actors. If you tell them their character feels guilty, they may have a hard time getting into character with that. To help them get into character, you use strong and emotional descriptions. Don't just tell them that they feel guilty, tell them what guilty feels like.
You pull the sword from the rack, and you feel as if your stomach sank into your feet. The sword, the walls, and even the air itself seems to judge you, and you hear their accusations echoing in the wind, Thief! Defiler! Unworthy!
Then, if they go along with it, give them inspiration.
Option 2: Dictate the full and complete effects of it to your players*
D&D has a lot of mechanics which punish players with heavy things (like dead characters) if they fail an encounter. This creates an expectation in some groups that player characters will, most of the time, cooperate and do what is best for the team, and anything else feels like a betrayal to the other players at the table.
Such players will not choose to act in a way that is against what they perceive to be the party's best interest. If you have such a group, present the complete effects of the control you are exerting, and make it clear what actions they are allowed to take or not take, and then leave them free to roleplay their character as they like in the space that remains.
When they fail the wisdom save, you say:
You are overwhelmed by inexplicable guilt. You put the weapon back on the rack, and back out of the room, and resolve not to touch the weapons again. You take 1d4 psychic damage from the lingering guilt even afterward.
Then, if they try to take the weapons again, do not let them repeat their save, instead, re-iterate the effect of the previous failed save, and make it clear that you won't budge.
You reach out to take the weapon, but the inexplicable feeling of guilt returns. No matter what you do, you cannot bring yourself to do it.
That said, you should only dictate emotions if they come from a magical source
In most circumstances, players are the final authority of their character's inner life. Dictating emotions or actions from a character without a clear external force acting on them is robbing them of their one and only source of narrative control within the game. Don't do it.
If you want them to feel guilty for a reason besides magical mind control, give them a reason to feel guilty, then accept however they choose to roleplay in the face of that reason.