Disney version; immensely underrated.
The 1970s version with, among others, Michael York, is probably the best version at the moment.
Mid-90s version with Liam Neeson as Valjean.
Polanski's version was good, for a straight take; the musical is quite fun, too.
The recent Robert Downey Jr. version is a very fun action-oriented take.
For more classical ones, apart from the BBC stuff that everyone recommends, there's a very good 1979 film called Murder By Decree starring Christopher Plummer as Holmes.
20,000 Leagues Under the Sea
50s Disney version.
The only film version that really comes close to the novel (that I've seen) is Kenneth Branagh's early 90s take; it's flawed, but worth seeing.