The single best thing you can do to raise an angel round is find the right anchor investor. Just like wolves and sharks, angels often travel in packs. There’s the Google diaspora, the Paypal mafia, YC alums, liquid Facebookers, the list goes on. Your challenge is to break into one or more of these packs and then get spread around like a hot potato. Win over an angel who is well connected with one or more of these packs, or co-invests frequently with a group of other angels, and get him or her to introduce you around. While it might take you some time to find your anchor angel, once you do it will pay off in spades. And at in the end the yield on your time will be much higher than randomly meeting with dozens of folks who might write you a $15k check.
So who are these uber angels who can get your syndicate filled out in a snap? Unfortunately there’s no master list out there, so you’ll need to do your homework. Angellist obviously is the place to start, but don’t stop there. Talk to as many founders as you can and find out if they had an anchor investor who brought in a number of other angels. Ask angels themselves. Be resourceful. And then, once you’ve built a list of target anchors, focus your time on getting to them.