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I would say start with thermal expansion. In the Unleashed pack you can do pretty much everything with TE. However, you need IC2 for jetpacks and a compressor. Like TE machines, quarries also take MJ. Having a good MJ supply early one can help speed up the resource gathering.
Thermal Expansion for sure. As much as I love the IC2 machines and it brings me back to my Tekkit days, most mods run off of Buildcraft MJ now and the pulverizer is much better than the macerator from IC2 because it can give you extra ingots from pulverizing. The very first thing you should start with though is Tinker's Construct