I've received a number of emails from users having trouble extracting files from team fortress 2 content.gcf. It's taken eight years, but with the advent of the TF2 Scream Fortress, Valve have finally authored a GCF file larger than 4 GB. As many of you have found out, HLLib does not properly support files larger than 4 GB (partly due to my naive younger self, and partly because I wasn't sure if Steam did either).
Long story short, I updated HLLib to support files larger than 4 GB tonight, and I will release said update this weekend when I have time to build all the installers and more thoroughly test everything.
Happy Halloween!
Update
HLLib 2.4.0, GCFScape 1.8.2, VTFEdit 1.3.2 and Crafty 1.0.2 have been released and all support GCF files larger than 4 GB in size.
New users can register here.