I reckon 'The Jungle Book' was the best. Great characters, animations and songs.
The trouble with all Disney movies of the 60s though, is all the liberties they take - mucking around with established stories and details (Sword In The Stone?). As well as crappy characaturing (sp?) of 'foreign' accents in order to appease some sample audience of ignorant burger chomping thickos who don't see much of the outside world.