I don't necessarily believe there is a correlation that winning the popular vote means if there were no Electoral College, they would have won the Presidency. The reason is, campaigns go in setting up strategy based on the rules of the game.
Let's use hockey as an analogy, since that is why we are all here on these boards.

A team built for the regular season (i.e., to win the President's Trophy, i.e., the Washington Capitals) is not necessarily a team built to win in the playoffs (i.e., the Stanley Cup).
Campaigns know that they are not going to win certain states. For instance, the GOP knows they will never win NY, California, or Mass. So, they don't care how much they lose them by since it's a winner take all system within the states. Thus, they don't waste their time campaigning there (other than to perhaps protect down ballot candidates).
Now, if they knew the popular vote was all that mattered, they would campaign in those areas that might swing either way -- like pockets of Upstate NY. Because now how much they lose a state is important.
So, when people go all angst on the popular vote being different than the Electoral College, I'm all meh about it. You have no idea how it would turn out if the campaigns focused only on attracting the popular vote.