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Are they hostile to you already? If they aren't I would try attacking their airport since they will have the most people there as sometimes their vertibirds don't count.
If they are hostile you have to go back and talk to preston and tell them that they're hostile or that you want them removed and that should do it. You don't get a quest about it until after the game, they're hostile and you talk to preston
I have tried killing them all at the airport but after i kill everyone there i don't get anything indicating that i should talk to preston, i have attacked them during the battle of bunker hill quest and when they drop off guys to fight super mutants i kill the guys they dropped off and the verti bird they came in (i did not save after incase killing them at the airport would have been just a waste of ammo and time but one time i belive they started having guys randomly walking around the wasteland that were hostile by default)
- killing any named character pertaining to the Brotherhood (e.g. Ingram, Kells, Maxson, etc);
- doing Institute's Mass Fusion instead of Brotherhood's Spoils of War, or relaying to the Mass Fusion building/siding with the Institute, while starting either or them;
- doing Undeground Undercover for the Railroad;
Once you are enemies with the Brotherhood, simply talk to Preston and ask him about taking down the Brotherhood.
Note: if you destroy the Brotherhood through With Our Powers Combined, you won't be able to loot some specific items, such as Maxson's battlecoat and his unique laser gatling gun.
http://fallout.wikia.com/wiki/Old_Guns