On my laptop, running 64 bit Windows 7 and with 2 Gb of free memory (as reported by Task Manager), I\'m able to do:
var x = new Dictionary
Update: The 2Gb single-object memory limit has been lifted on 64 bit with the release of .NET 4.5.
You'll need to set gcAllowVeryLargeObjects in your app.config.
The maximum number of elements in an array is still 2^32-1, though.
See Single objects still limited to 2 GB in size in CLR 4.0? for more details.