Settlements. Make it your mission to turn every workshop location into either a large community that offers all services, or a smaller homestead/outpost for the people currently living there. Develop them all.
There's a ton to do even if you have beaten every quest available. Collect all bobbleheads, magazines. If you have the corrects saves you can go back to a point where you can side with another faction so you can try and get all the achievements. There is probably more, but that's all I can think of off the top of my head.