Why the symmetric key layer in PGP? I've been familiarizing myself with the basics of PGP. If I understand correctly, PGP symmetrically encrypts the data of interest using a random single-use key, then encrypts the encrypted data and its symmetric key using the public key of the intended recipient.

What benefit does the inner layer of symmetric key encryption provide? I am having trouble understanding how this layer adds security over simply encrypting the data with the recipient's public key straight away.
I think you misunderstood a detail of PGP encryption. Only the random symmetric key is encrypted under the recipient's (asymmetric) public key. This way to encrypt stuff is quite common and is called KEM/DEM paradigm: Key Encapsulation Method/Data Encapsulation Method oy Hybrid Encryption. Some refs: en.wikipedia.org/wiki/Hybrid_cryptosystem and en.kryptotel.net/encryption.html.