Dispite the extra content of the PS2 version, I really think the graphical difference between the two is big enough that you should get the GCN version. RE4 is all about immersing you into the world of the game and it does a great job of doing so. While the PS2 version still looks good, it doesn't look nearly as good as the GCN version and this really affects how much you are sucked into the game. Some areas have negligible differences (less foilage, particles, etc), but some places are like night and day. Any area where there are a bunch of villagers coming after you, the villagers look pretty bad. Their face textures are blurry and look two dimensional (they remind me a little of the faces on the characters in GoldenEye and Perfect Dark). Also, there are a few scenes that take place at night with lightning flashing in the distance, lighting up the scenery. These sections look more impressive on the GCN than the PS2, and gives you a much more intense feeling of creepiness. When I first played the PS2 version, and I saw what it looked like, I couldn't get passed how it looked and didn't touch if for a week or so. The load times are also a bit longer on the PS2, requiring for a 'Loading' screen between area transitions, which also temporarily removes you from the world of RE4. The cutscenes on the PS2 are also pre-rendered, while they run in real-time on the GCN. This means that if an object is destroyed in the background on PS2, it will be back again in the cutscene. It probably also means that the characters will always be wearing their normal costumes in cutscenes even if you are wearing the alternate ones in the game. This is yet another thing that slightly jars you out of the 'reality' of the game. In the GCN version, what you see while you are playing is what you see in the cutscenes. I also find that the GCN controller seems a little more intuitive and responsive. I guess it's also worth mentioning that the sound on the GCN version sounds a bit crisper, but it's not a big deal.
The game is, of course, excellent on both consoles. By now, the price of the GCN version of RE4 has dropped quite a bit and you can pick it up for about $30-$40, and sometimes less. The MSRP of the PS2 version is $40. I don't know if you can find the collector's edition of the GCN version anymore, but I assume it's still going to go for about $60. The PS2's collector's edition (actually called the 'Premium Edition') may be a bit easier to find and goes for $50. As far as packaging goes, I like the PS2 cover a lot more and the content in the collector's edition for the PS2 blows the GCN version away. The metal case for the PS2 set is much nicer than that crappy 'GameStop' version GCN owners got, and it also comes with a bonus 'Making-of' DVD. Besides the bonus DVD and the case, the only difference between the contents of the 2 collector's editions is that the GCN one comes with a laser cell of Leon while the PS2 one has one of Ada. I'm an Ada fan myself, and that picture of her is really sexy, so I like the Ada one more.
So yea, that's my take on it. The extra levels/costumes on the PS2 are great (I love that there are new missions where you can play as Ada!), but for the main game, the GCN version is simply superior. The graphics are just THAT much better on the GCN. Normally, I don't really care about the graphical differences between ports, but in a game like this, where the atmosphere is so important, it's hard not to notice the shortcomings of the PS2 port. For those of you that think I'm just being picky, just play through the first section of the PS2 version, up until the church bell rings. Notice the look of the villagers (especially their faces) when you are playing, and then compare them to the faces of the villagers in the cutscene. It's a huge difference! The GCN version has the villagers looking like the cutscene throughout the game, and it really helps to look at some detailed, freaky looking guy rather than one that looks bland when you are trying to get into the game. Of course, my complaints might just stem for my playing the original GCN version, then switching to the PS2. Maybe if you've never played the GCN version, you won't be able to tell the difference.
My recommendation is for you to get the GCN (regular) version first and play that. Then you should pick up the PS2 Premium Edition if you really liked the GCN version for that extra DVD and the new content. If you just want to toy around with the new costumes/weapons or want to play the new missions, and don't want to purchase the game again, just rent the PS2 version.
Anyway, here's a short list of what I think are the pros and cons of each version:
GCN:
++Much more immersive
+Better graphics
+Real-time cutscenes
+More intuitive controls
+Faster load times
+'Crisper' sound
-Ugly packaging for Collector's Edition
-Two discs (swapping discs is a little annoying)
PS2:
+New weapon
+New missions starring the ever-sexy Ada Wong
+New costumes for Leon and Ashley
+Making-of DVD with the Premium Edition
+Box for Premium Edition is very nice
+Single Disc
+Sexy Ada cell with the Premium Edition
--Not as immersive
-Slower load times
-Worse graphics
-Pre-rendered cutscenes
-Sound is slightly muffled (a little noticeable with the dialogue)
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