I threw in some video links for how they sound as well. Good thread!
Four Cylinder - F20C
I must give credit where credit is due. I'm not a huge fan of Honda, but this is quite an amazing engine. Revs for days, 120 bhp per liter with natural aspiration, and it's absolutely bulletproof. There is probably a better engine than this built by Honda, but my knowledge of Honda is rather limited.
Six Cylinder - Arese V-6
Now my bias will show. It's an absolutely beautiful piece of machinery, it sounds incredible, and it was making more power than most V-8s of its time. Did you know Alfa Romeo was the first company to use variable valve timing in production cars? Two other engines I must mention though are BMW's straight-6 engines. No explanation needed...they've used the same design for decades on end and it's never failed them. Also, Porsche's flat-6 engine for the same reason.
Eight Cylinder - Rover V8
The LS series has already been mentioned, so I thought I'd call attention to the Rover V8. This was originally a General Motors design, the Buick 215 engine. It was extremely efficient and quite light, but it was a rather expensive design and it would've been scrapped until Rover bought the rights to the engine and redesigned it. This engine has been used in cars built by Land Rover, TVR, Morgan, and Triumph and has even been used in some light aircraft. It's like Britain's version of the Chevrolet Small Block.
Ten Cylinder - V10 TDI
I like diesel technology and I was blown away by this engine when I saw that it delivered 500+ pound feet of torque and still managed to deliver 25 mpg on a vehicle that weighs 5000 lbs. I don't even like SUVs, but I would buy a Touareg just for that engine.
Twelve Cylinder - AMG V12
AMG has taken the smoothest engine configuration and has turned it into a nuclear weapon. While I like the twin turbo rocket sedans by Mercedes that feature this engine, my favorite application is in the Pagani Zonda Cinque where, in naturally aspirated form, it makes nearly 680 bhp. That's just mind-blowing to me.
Sixteen Cylinders - Bugatti W16
Yea there aren't that many sixteen cylinder engines out there, but I have to call attention to the W-16 which I think is an engineering masterpiece. It's one thing to get 1000 bhp from an engine, but it's quite another to get it in a production car that can be driven daily...oh, and it sounds like a Blackhawk helicopter. Amazing.
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