Even that change would require a constitutional amendment. Article II, Section 1 specifies that the method for appointment of electors is to be determined by each state's legislature.
States are already free to do what you propose. I believe that there are two that do. The states can't, though, be forced to do so without an amendment.
A constitutional amendment is the proper mechanism. If a few states changed, it could radically alter the results. California and New York could hand the White House to the GOP by switching to a district by district allocation. If a few large conservative states switched, it would hand the White House to the dems.