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Ancient Blood Angels player here, and I've always felt it sacrilegious to Ally in regular Space Marines; however I am going to do it soon simply because I want to fully test out these new super-wacky psychic powers with a ton of Librarians.

So if I run a Blood Angels Baal Strike Force (CAD)... can I ally just the "Librarius Conclave" formation? -- or must I first ally a proper SM force to add the formation to?

You can ally in just the LC formation.

Formations are detachments. Taking a librarius conclave is now no different to taking combined arms detachment as far as army composition is concerned. They just benefit from different special rules.

Basically, the formation is the modern equivalent of the "SM force"

Thanks gents.