I would guess there is some way to block PayPal by contacting your bank. But that still leaves them your account which they will use to pretend they have customers.

You can still remove payment methods but you cannot delete your account

I literally just tried

I had to remove EVERY SINGLE vendor I had ever paid from some stupid list that evidently gave them the ability to automatically charge me (thank God I keep track of shit) just so I could remove my bank account

But there is no option for me to delete the account wholesale