It seems that the popular press, and even election discussion forums like this, when discussing changes to the electoral system start with a presumption that popular vote needs to somehow be weighed more.
I think just the opposite. The nation is a collection of states. The states chose to join the union, and in an act of compromise, the small states agreed to cede some power to the larger ones in the house of representatives. But other than that, and the related electoral votes, each state is an equal partner in the Union. When it comes time to pick the president, each state chooses its electors in the way it sees fit. Currently, all states use a popular vote method, but there is no reason that will always be the case.
In any event, with the significant influence a few large states have (it now takes just 11 to win the presidency), I believe real consideration should be given to limiting the power of states like California. One state=one vote (similar to the UN) would make sense for the selection of President, though I'd still keep the house of representatives based on population.
If the concern was that the large states had too much power by winner-takes-all and the small states that have disproportionate electoral weight, then you are really arguing for a more balanced population between states. Presumably that would be to help mid-size states. If that was the goal, the Constitution would have provided for representation penalties for states that were too small to encourage merger, and for those states too large to encourage splits.
