According to this page – http://www.musicweb.force9.co.uk/music/railways_in_music2.htm – "Puffin' Billy by Edward White [was] inspired not by the old Northumbrian locomotive but by a small engine seen on the Isle of Wight, a movement once used as a signature tune for BBC Radio's 'Uncle Mac's Children's Favourites.' "
Here's a site that offers lyrics to a couple of songs that were featured on the Captain Kangaroo show, but no lyrics for the opening theme: http://www.streetcarmike.com/kangaroo.html