How to Quickly Get a Sim Enraged?

Give the sim the hot-headed trait, use angry paintings and a selfie taken when angry and just make sure you don't have things around that give them "happy" moodlets to counteract it (like decor, clean laundry, etc.)
There's also a recipe for making sims angry which a sim can make at cooking level 4 if you get them angry and a drink at mixology level 2; preparing those ahead of time will allow you to stack onto angry moods to help counteract any positives.

If you have Spa Day, do something for a few hours with the sim ahead of time that gives them the ability to surge emotions, which lets you pick the emotion you want the sim to enter. Painting works well for this.

Have the sim pursue the acting skill/career, and they can get angry by choice at will.

Seeing as you are just trying to tell a story, one thing a lot of simmers also do is use UI Cheats extensions so they can right click to remove the mood buffs they don't want.

My high maintenance sims love to die of rage.

I have a mod (which I am not allowed to discuss). Basically, my sim woohoos with a married sim's wife right in front of him. I've had 3 die of rage so far....

I use a mod called Storytelling Socials that adds a lot of fun social interactions with moodlets. I've had Sims cheat and get into an argument and use mean socials from this mod that led to death by anger very easily... sometimes accidently.

I suggest the mean vibe lot trait.

Get the emotionally mindful to "fine +10" and have him surge anger.

Get into arguments. Get cheated on.

Hot head and high maintenance are great traits to have for anger.

Have him dislike something and then force him to do it.

Dislikes cooking and holiday music or whatever. Turn on the radio and force him to cook. That'll usually turn from tense to anger.

In addition to what others have already shared, if you have the Digital Deluxe upgrade, it came with 'Awesome Animal Hats.' There's an Angry Lion hat your Sims can wear to get angry. Also, if you had TS3 and got the emotion lights/lamps, I'm guessing there might be one for anger. I never played TS3 so I'm not sure about that one, but thought I'd mention it. :)

Also, I saved this link to a thread on Carl's Sims 4 website a long time ago that has come in handy to me many times. It gives a list of every emotion and how to get your Sims in that emotion. It's an old thread though with mostly ideas to use from the base game, but thought I'd mention it anyway. :)

Emotions and Items/Actions That Influence Them

Remember this? ?

https://forums.thesims.com/en_us/discussion/998469/how-to-quickly-get-a-sim-enraged

I figured you had. First thing I do when someone asks a question is to Google it. This time, as has happened in the past, it lead me right back to the forum. ?

I did originally kill him with rage via MCCC by adding the enraged moodlet but it says underneath "You cheated to get this moodlet" and the death didn't seem natural for the story.