Tough call this as I am not massively into u2's eariest records - TUF is a stone cold classic, a fantastic record which I love, but the rest are just OK in my book.....I was never much of a Police fan though so U2's 5 edge it for me.
As an aside I think both bands early albums fall short of Echo and The Bunnymens first 5 in the quintessential early 80's album stakes though.
The Bunnymen never kicked on after that IMO - but Crocodiles, Heaven up Here, Porcupine, Ocean Rain and Echo and The Bunnymen trump both u2 and The Police's first 5 in my book.