Power - There was one, but it got cut from the game. I guess it would be a combination of fortune and popularity, with a focus on politics, law military careers.
Creative - This would be focused on the more artistic endeavors. Careers would be music, entertainment, cuisine, perhaps slacker
Deviancy - For your more antisocial Sims. Sims want to pick fights, get a bad reputation, and soap fountains. Main career would be criminal.

Not sure what it'd be called .. but somethin along the lines of a naturalist .. someone who prefers do green and such as much as possible

We used to call that Granola. I don't mean that as a put-down, though. Please don't take it as such.

Absolutely second creativity and power. I also wish TS2 had an alternate romance aspiration akin to TS4, I know family kinda works like that already, with its emphasis on marriage, but family also emphasizes having kids, I wanna focus purely on the aspect of romance and nothing else; a sim trying to find their soulmate, a sim who likes trying different ways of woohoo, a sim who likes going on dates. Maybe call it the Passion aspiration; career wants for things that people are generally passionate about, i.e. the gamer, journalism, law, and even criminal careers.

I'd also like two Knowledge aspirations. One for the supernatural stuff, and one without.

Hmm, sub aspirations might be cool. Romance as it is now or committed and romantic. Knowledge as it is now or focused just on learning ordinary stuff.

Maybe some hybrid of knowledge and romance for hippy sims. Spirituality maybe? It being a Sims 2 aspiration, it'll have a tinge of parody by playing into new age-free love stereotype. Careers could focus on university careers, especially the paranormal and natural scientist career tracks. The want tree would include declaring philosophy as a major, yoga, meditation, woohooing x amount, "blowing bubbles", becoming a plantsim, and other hippy desires. I think fears would include getting a job, going to private school, dead plants, buying clothes, etc.

Name it 'Hippie.'

In Oakbrook, I played Lazlo Curious and his wife as something like that. They had plants everywhere, and Oriental-styled furniture, and wore robes (or maybe kimonos, would need to check) and long hair.

The more I think about it, I like the Deviancy aspiration. But not just for bad sims, but for their opposites - the vigilant heroes. I think it would really suit sim versions of superheroes, to go around fighting crime and get happy doing so, solving intricate plots and whatnot. Put soap in that fountain! So the main careers would be Criminal, yes, but also Law Enforcement, so that superheros and supervillains of each respective track could have glorious battles with tons of collateral damage.
Now that would be a good aspiration for many of the residents of Veronaville! To better encourage war rather than peace!

In Oakbrook, I turned all the Capps into vampires and the Montys into werewolves. It was fun.

False Graded - For unlucky sims when they study a lot, they'll get an F grade.

Edit: I thought this was TS3, I am such a blind bat xD

Useful?

Sally Sims wants to lead a useful life, making her own life and the lives of those around her better. She will need Creativity, Charisma, a new skill called Patience and has to study Anger Management.

When Sally reaches the top of Usefulness, she will be in Platinum forever.

(Okay, I just appreciate useful Sims, and can sometimes do with more of them in my hood )

How about Philanthropic or Do-Gooder? They like to do good, give to charity, maybe adopt orphans, work in fields like Medicine and Education.

Useful - not working in a field, see? Be useful where you are. You can do that in or without any career.

"Do your little bit of good where you are; it's those little bits of good put together that overwhelm the world." (Desmond Tutu).

I think one that would suit The Sims is Adventure. They like to travel, experience new things, visit new places, go hiking, court danger, join the Adventure or Military careers.

Another one I've thought of: Philosopher-some who isn't really into working, but day dreaming, making toys, just goofing off. They often don't have any careers in mind, and they're more goof offs than anything.

Procrastinator - will suit lazy Sims

Something akin to a Pleasure aspiration, but more heavily focused on playing the videogame console, the computer, or even playing the arcade machines. One of the big career LTWs would be, of course, the gamer career.

I agree with the 'naturalist' suggestion. Something focused on the gardening aspect of the game, like more frequent wants to plant new seeds, harvest produce of certain quality. Maybe even an LTW of 'Grow every type of crop'... which likely would include a revamp of the gardening system, to add stuff like more seed types to grow, cross-breeding. Or even growing a cow plant. (Wasn't that last one an LTW in Sims 3 or 4?)

Similar vein, some kind of 'handyman' or 'crafty-craft' aspiration focused on using the OFB benches to make pottery, flower arrangements, or focused on building toys/robots.

dabbler/ inventor - likes to do things hands on
hoarder - wants to buy any and all sorts of deco and loose points if things are sold/ stolen/ or not bought/ got in a certain time

I think we already have these things. The use of the trait mod allows for serial romancer or hopeless romantic. For a naturist you can use the echo friendly and vegetarian traits and have them live off someplace on a farm. Much of it is just small mods + some imagination.

Pleasure sims are easily balanced out by adding a secondary aspiration.

I don't use the traits system/ mods (whatever it's called). When I heard of it I thought it was a cool idea, but when I actually looked them up the what needs done and all that jazz confused me so I passed on usin them

I considered it, but figured I'd end up spending too much time resolving conflicts. The extra LTWs mod was already enough of a pain to get in (though working smoothly as far as I can tell).

'Letmebe' for lone or distanced 'antisocial' sims.

There aren't that many conflicts with other mods that I can tell-the traits themselves are independent of any other mods, and who ever makes a mod that uses the traits always checks to see if it does conflict with another trait.

I find them useful at times. Although I'm afraid that I have a higher than normal number of insane or unstable pixels in my neighborhoods...