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Unlimited Spells is a perk that removes the limited-charge from many limited-charge spells, allowing them to be cast infinitely many times.
Tips
It is a very powerful perk early on in a run, as it allows for dealing way more damage than by using the regular spells you have access to. However, it can also help salvage a longer run when you haven't been able to build a strong wand capable of carrying you to victory.
This perk enables easy and effective digging through most hard materials using an appropriate bomb-like spell, except for Steel and Extremely Dense Rock which will only be destroyed by the explosion from Nukes or Holy Bombs.
Synergies
Coupled with the Bombs Materialized perk, you can cast infinitely many bombs from your item slots, either for digging or practically as an extra wand.