Depends what you want it for. If you're going to be in a support roll in a team, buffing sets like /kin and /emp are the best way to go. Typically these are coupled with Illusion since Superior Invis allows you to be invisible and fire off your buffs at the same time. Grav/emp is pretty nice too, since you can basically drop your singularity and then allow that to do the controlling for you while you buff/heal the rest of the team.
1vs1s, grav/rad and fire/rad are the best overall, with ice/rad being very nasty at 50 (with epic blast). Basically anything /rad is the way to go for duels, with grav and fire being the best two sets overall.
General annoyance, go with mind/FF, ice/storm, grav/storm, anything /TA.
If you do more baseraids than anything else (but I don't think there's anyone who rolls a toon specifically for baseraids), earth/ff and earth/storm are nasty.
If I knew a bit more about what you were planning on using it for, I'd be able to give better advice 
well at the moment iv got a mind/ta controller and pvp wise its very very strong, you'll be able to survive and hold your own against basically all the alts apart from a stalker *unless you have tactics* so yeah thats the sets i recommend. Nothing better than slowing your opponent *glue arrow*, debuffing them *acid and poison gas arrow*, the 3 holds *ice arrow, mesmerize and that other mind 1 lol* and the panic button in case they get within strikin distance . . . . telekenesis *one of my fave pvp powers *
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Despite lot of moaning after the epic damages, I think controllers are still quite good. For a duel controller I guess flavor of the current month is almost anything /rad , except earth. Particularly grav, fire or maybe ill. I think /storms still ok too.
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*, the 3 holds *ice arrow, mesmerize and that other mind 1 lol* and the panic button in case they get within strikin distance . . . . telekenesis *one of my fave pvp powers *
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Dominate is the hold, mesmerize is the sinle target sleep and im guessing you mean total domination for the 3rd hold although being AoE means its pritty damn rubbish for PvP sadly 
As for TK cant go wrong there 
However if you plan on using this a lot make sure to get a secondary that gives you a nice end recovery like /rad, /empathy and /kinetic's (although a little harder to use since your target is being repelled away from you and out of transferance range)
As for primarys i also suggest illusion, grav and fire since they all seem to be standing up well during this horrible time of nerf's
I've used two trolelr types in pvp being an Ice/Storm & Grav/FF
Both of these prob would go under the annoying sets. Now if you don't want to feel like a squishy really go for FF the annoyance of PFF up constantly and Force Bubble can wreak havoc at high levels. However it won't help you take down your opponent too well.
For dueling */Rad is very good with mean */Storm builds too. Msot trollers can PvP pretty good regardless of sets but for a fav I'd actually say */TA more of a support in a team and taking on large group of opponents in zones/base raids/ team arena but great powers to have!
What sort of PvP did you have in mind?
Dunno, tbh, I suck at PvP as Spawnus will take great delight in pointing out, I just want a toon that is fun to play in PvP, really
We built this city on Rock and Roll!
Im have a troller im building 4 pvp, im going 4 ill/rad, i have faced some trollers and the ill/storm and ill/rad is the most nasty i have faced, i havent faced grav, fire or TA yet tho.
Friend of mine has lvl 50 ill/rad and i have never seen him lost to any AT yet in 1vs.1 , but like some other say here, there are many nasty sets 4 trollers.
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Dunno, tbh, I suck at PvP as Spawnus will take great delight in pointing out, I just want a toon that is fun to play in PvP, really
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Yes he Sucks at PvP, getting killed by a Fire Tanker 
Now I know that I'll get a million different answers to this, but I wanna roll a Troller for PvP and was wondering what's a good pair of sets?
Make some comments and suggestions and I can base my choice on what I fancy then
Are there any FOTM's atm?
We built this city on Rock and Roll!