I always go for an alliance with the Papal States as early as possible. If you don't get him in your gang then you can bet that another Catholic faction will.
When playing a diplomatic game I'll recruit 4 or 5 diplomats as soon as possible and send them to the four corners of the map and one to Rome. In the first few turns I try to meet as many factions as possible getting trade rights, map information and importantly alliances.
The more alliances you have, the more valuable your allegiance will be to others meaning you can lever high tributes or even provinces out of them because they'll want to be with the gang.
By the time you reach the Pope, you'll probably already have several alliances under your belt so he'll snap your hand off when you offer him an alliance.
When you've got all the Catholic factions and the Papal States in the gang, then you're in a good postion to screw huge penalties out of anyone who attacks your lands. A ceasefire will cost them one, two or even three provinces and or crippling tributes.
That aside, one good trick you can pull with a Papal ally is if one of his armies is next to another Catholic army, attack the other army with your own stack. The Papal stack will automatically join the ruck leading to the other faction entering a state of war with the Pope - instant excommunication for them and that faction's lands are then fair game. Happy days.
It works with ships too, obviously.
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