And would still have to download from their source.
Serving up that large of a media library at mid scale just isn't really a great use case for a CDN, those that have to due to transit costs becoming truly enormous (e.g. Netflix) make an enormous investment in hardware at the edge that probably isn't affordable to IA (or necessary at this point).
Also, since archive.org has so much content, the caching ratio is going to be very bad and kill CDN efficiency while still requiring lots of direct bandwidth. Cheap direct bandwidth in their case looks best(which is what they seem to be doing).
The way they use bandwidth means the most efficent GB/dollar cost although at the cost of poor performance.
Forgive me, but what is an AS?
An AS is an entity significant enough to be reasoned about at the BGP level.
If they wanted to use Cloudflare, I'm pretty sure they'd jump at the opportunity.