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No Merchant -- Very popular with classic survival horror fans. Not having a rifle is sometimes a bigger challenge than not being able to upgrade your stuff. Default attache case is also a major factor in this. You can make it even more like the classics by avoiding enemy drops (only collect items that you actually find inside the levels), and by only saving on typewriters (gets pretty intense when you have to do several rooms in a row without saving/continuing).
Default Handgun Only -- You can only use the Handgun that you start with. Upgrades are fine, not only 'cause it's more fun but because otherwise this is just a more restricted No Merchant. I also allow knife and grenades.
100% -- Collect all treasures and bottle caps, max out Leon and Ashley, fully upgrade the weapons you're carrying, etc. Basically this is the 'leave nothing undone' run. I did this a couple years ago and I was surprised by how many rooms and items I didn't even know existed. As a sub goal, set a number of kills to have by the end. I think 1,000 is challenging enough without being unreasonable.
Glitch Run -- This is way more fun than it sounds. Google RE4 glitches and see how many you can perform. Some glitches give you a ridiculous advantage (like double speed and the ability to skip rooms by going out of bounds). You can also use the TMP to shoot padlocks from the other side. All these glitches are used in speedruns, so it might be even more interesting to add a goal for beating the game under a certain time.
Assignment Ada 100% Kills -- This extends AA by a fair bit. Just kill everything. What makes this unique compared to the main game is that in AA you don't get a knife (can't upgrade stuff either). Gotta be extra careful with supplies if you want everything dead at the end.
My Super Mario Maker levels ~ https://supermariomakerbookmark.nintendo.net/profile/Ren_Dood