Personally, I think Sentry’s Sacrifice to death is fun and spot on. Ares does the same thing.
OML can do it too if you’re not careful!
But those one’s are pretty obvious.
I think my new all time favorite one is now when the Lieutenant drops his yellow heal tile and 3* Strange blasts him to death for his troubles.
What’s your favorite?
Yep, I was going to give the general ‘Death by Strange’ but when the Lieutenant does it, it’s particularly satisfying.
Though it’s not completely fair to describe it as suicide, I giggle whenever the AI makes a red match that triggers Daredevil’s sausage drop skill.
Ragnarok finishing off his entire team with Tinykittylike Power can be amusing, but usually it just seems like a bird flip on his way out the door.
I also have had my own incredibly powerful 1/1/0 255 Blackbolt kill himself by energy channeling, which amuses me more than it probably should "Fear my energy channeling, human, lest I **ooohhh what a headache ahhhhhh thump **.
Any AI suicide that isn’t the result of my characters taking high damage like an over-levelled headbutt or sunder is fine by me. 
This would be nearly impossible to pull off, but what would be fantastic AI suicide:
All on the same turn:
Sentry casts Sacrifice, kills himself. OML damages himself to near death.
Hulkbuster casts overdrive, kills himself. OML damages himself again, and kills himself.
This has MPQ: The Musical written all over it. Hamilton, your time is done!
Juggernaut Headbutting while he hasn’t got enough health is my favorite
especially if he headbutts a character with regeneration
The black arts countdown from the hand. Hurts a teammate and heals himself. Leave him alone with full health and all he does is take out his buddies for you. And while it doesn’t hurt them, I love when the AI uses a board shake ability that messes up a match 5 they would have made.
My favorite is during the Quicksilver Versus event. AI Quicksilver matches blue when there are 3 charged tiles on the board. His passive triggers and adds a 4th blue tile. My passive triggers and kills him and his team.
Death by Dr Strange is also bringing joy into my life every day now.
I also have had my own incredibly powerful 1/1/0 255 Blackbolt kill himself by energy channeling, which amuses me more than it probably should "Fear my energy channeling, human, lest I **ooohhh what a headache ahhhhhh thump **.
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I am obviously playing this game too much because I just about laughed myself off my chair at that one.
Thanks, Moose.
My favarite is when the AI gets a massive match-5 cascades. Oops, JG is on my team. 
Having enough protect tiles out for juggernau’'s headbutt to do very litre damage to my team but kill him. Also like sis new power to turn team invisible would be funny to watch suicide headbutt an invisible team.
Not AI, more of my own suicide but back when sentry-bombing was a thing, he could KO both teams and you would still get the “W”. Wasn’t good for health packs but for some reason I enjoyed winning by downing everyone on the board. 
Death to all 
Daken. I tend to leave self-healers until the end so I can down them with a barrage of attacks. I tend to leave healers till the end, and I’ve had some matches where he dies the turn after I finish with the first 2.
This overlaps with what some other people have already said, but having Sentry cast Sacrifice and having Dr. Strange retaliate with flames. Hah, I really did think that finishing fight would take more than one enemy turn to win 
Goon #1: “Look, it’s Dr. Strange! Drop some covering fire.”
Goon #2: “Okay, I can do it in 4 turns… oh no, that really hurt goon #3!”
Goon#3: “No problem, I can drop a countdown that will heal… uhn!”
Goon #1: “Crap, goon #3 is down. That Dr. Strange is nasty! Obviously I need to drop two countdowns this turn, that’ll get hi…”
I still get a chuckle out of Ares Sundering himself to death.
And now that they finally fixed his Yellow Countdown tile going away when he dies (I THINK it’s finally fixed for real), it’s even more humorous.
D3adpool. Love watching him try too hard to be the Life of The Party.
Also not technically suicide, but I’ve had more than a few PVP matches against Black Bolt where I match the most of the charged tiles myself, and down his entire team with like a fraction of the moves it would usually take. Not sure what keeps making people think a single-covered energy channeling is good enough, the AI sucks at going after those charged tiles.
My favorite was the last Sentry PVP where Quake was boosted.
Yes, please nuke your team into oblivion while I take 1. Rinse and repeat.
I thoroughly enjoyed playing Vision against Bagman in DDQ last week (I think). I made a couple of blue matches, cast blue, and Bagman kindly kept my countdown alive for the rest of the match. I may have made “bam”, “kapow” type noises, I couldn’t possibly comment.