Various themes in the culture of Catholicism make it easier to be charitable because they help Catholics avoid the rational arguments that would discourage them.
The most difficult hurdle to giving to a charity is determining if the charitable gift is worthwhile. Will the gift do enough good? Is the charity deserving? Are you just enabling poor people to stay poor? Catholicism by-passes all of these rational arguments with irrational beliefs*. These beliefs may not be universally held, but I believe they are part of the culture:
(1) Sacrifice is a good thing in of itself. Value is placed on the sacrifice itself, not just the good that comes out of the sacrifice. Thus the giving Catholic doesn't have to worry (as much) about whether the charity is really deserving.
(2) People in need have an elevated status. No need to argue within oneself about whether poor people deserve help and no need to weigh their utility function with your own -- as a Catholic, believe that they deserve the money or time more than you do.
(3) The reward is intangible. You don't need to expect or require that there will be an immediate benefit as a result of your charity. This prevents discouragement when the charity doesn't seem to be working.
Any person who gives to charity may hold any of these beliefs to any extent. I would bet that the more rational a person is, the more good they will do with a given amount of money. However, it is the irrational components that are probably most responsible for the amount of money that is given -- and the more money that is given the better, perhaps. Even though some money is wasted, there's more money going to the worthwhile charities as well.
*You could argue that the irrational beliefs are just assumptions that are made in the game. There may actually be rational arguments behind them, but the belief is a short-cut because the arguments need not be constantly re-examined, especially by the set people who are not interested in arguments.
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The reason Catholics are better organized than humanists is that they're official, communal, and hierarchical and we're not. The reason cults are better organized than Catholics is that they're even more official, communal, and hierarchical.
If the Pope says "Donate ten percent of your money to me," then there's an expectation that ordinary Catholics will obey. They've committed to following what the Pope says.
If you, Eliezer, posted on this forum "Please donate ten percent of your money to the Institute That Must Not Be Named", well...actually, I don't know what would happen. A few rare people might do it to signal that we liked you. But although we often follow you, we are not your followers. We haven't made a committment to you. We associate with you as long as it's convenient for us, but as soon as it stops being convenient, we'll wander off.
If you really want to get an infrastructure as powerful as the Catholic Church, you need to ask us to officially swear loyalty to you and start publically self-identifying as Rationalists with a capital R (the capital letter is very important!) You need to put us through some painful initiation ritual, so we feel a commitment to stick around even when the going gets tough. You need to make us publically profess how great Rationalism is to all our friends enough times that it would be a major social embarrassment to get kicked out for not obeying you enough. You need to establish a norm that following Eliezer's requests is so completely expected it would be strange to refuse and we'd be going against all our friends. And then you need to keep telling us about how much better off we are as capital-R Rationalists than as members of the boring old general public. Then you can start ordering us to donate ten percent of our income and expect Pope-level compliance rates.
The cultists do all of this, and the Catholics try but generally fail, which is why many Catholics don't listen to the Pope nearly as much as atheists think. If you didn't want to go quite this far, even making us pay $5 for a (physical, laminated, colorful) Less Wrong membership card would probably make a difference. Once we did that, we'd be members of something, instead of people who came to a blog every so often to discuss an interest. The brain cares a lot about this sort of thing.
[edit: better explanation below in response to ciphergoth]
I like your points about what makes an organization have influence over its members, and I think you are spot-on about the different ways that are effective in creating group cohesion. However, I don't think that Catholic charity is so much mandated by the church as a rule or even an expected behavior as it is a product of the culture. When Catholics give to charity, it feels like an individual and optional choice. Whereas going to church and not using birth control may feel more like following the rules. I think there is a difference between behaviors that are done to identify with a group verses behaviors that done because you identify with that group..
The analogy would be rationalists doing something rational not because they're told to, but because they believe in rationality. That's why they're in the group in the first place.