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For reasons entirely aesthetic, I want to run an alliance of Stormcasts and Sylvaneth. I don't particularly care if those armies synergise well or not, my question is simply about which battle tomes I should acquire. I know books aren't technically "necessary" in Age of Sigmar, but I feel like I'm missing out by relying only on warscrolls, and besides, I usually spend a lot of time just reading through GW books just for entertainment, so I don't mind the investment. My question, though, is can I pick up both armies' battle tomes and still run them as a grand alliance, or is the grand alliance book itself a better option?

Skip the grand alliance book; it is outdated. Get the Core Rulebook for access to the Grand Alliance: Order. The Sylvaneth battletome will allow you to run the "Guardians of Alarielle" battalion which lets you run a handful of Stormcast units within Sylvaneth allegiance (and you can still ally in on top of that).

Agreed the Grand Alliance books were mostly released when AoS first got sensible rules and are quite out of date now.

The Big Rule Book gives you the alliance abilities, core rules, battleplans and also a nice chunk of meaty lore to read up on.

The Sylvaneth Battletome gives you all the lore and rules of the Sylvaneth along with their battalions (of which one, as said, features Stormcast). In addition it will give you all the options and lores to run that faction on its own as well. So you can vary between a full grand alliance force or Sylvaneth with stormcast allies.

Stormcast Battletome is the same, only it won't have a dedicated Sylvaneth battalion. Otherwise it gives you a good background and core for the Stormcast as well as all the warscrolls and such and, again, lets you run a stormcast force with Sylvaneth allies.


In addition you'll want to pick up the Generals Handbook 2018 for and updates it gives to either force (most likely on the syvaneth). The main difference is that battalions went up in points with 2.0, though you can get those details from the free warscroll builder on the Warhammer Website.
https://www.warhammer-community.com/warscroll-builder/


So that's two Battletomes and the Big Rule Book and the Generals Handbook 2018. In addition if you are doing AoS now you'll likely want to pick up the Malign Sorcery boxed set, both for its book and the models for Endless spells. Note that the book in that doesn't contain many rules, but it does contain all the realm artifacts and lores and such that you might well need if you like/your area uses realm abilities. So that book is more of a "pick gear and note down its bonus on your army list" rather than one you need to consider consulting game to game (like the rules or stats for armies).

Thanks for the info guys. I think I'll go with the core rulebook and the battletomes for now. GHB and Endless Spells may come later or I may try to share a copy with someone else, but for now, the first three should be plenty.