The '60s were the heyday of instrumental hits, and a lot of them came from movies. Here are two that are instantly recognizable. Ennio Morricone's score for The Good, The Bad, And The Ugly features whistling (another lost art), wordless grunts, and amazing surf guitar. Francis Lai's theme to Un Homme Et Une Femme (A Man And A Woman) isn't technically an instrumental, but the vocals are just nonsense syllables, so it's close enough.
The movies are pretty good too.
Ennio Morricone - The Good, The Bad, And The Ugly (Main Title) Francis Lai - A Man And A Woman