I think Trafficante. Santo was big in Cuba, as big or even bigger than Meyer Lanksy. He was at the center of the anti-Castro efforts by the CIA and the mob. He was huge in heroin, in fact he traveled directly to Asia to open up that pipeline(another joint CIA/mob venture). And even though he had a small family he had a lot of people/territory under his umbrella, he ran numbers with the "cracker mob", bolita and drugs with the first wave(pre-Mariel) Cubans etc.
No way to compare them when it comes to money because it's impossible to know how much they made*other than the absurd $2 billion/year figure from the Marcello book) but in terms of status the things I mentioned above give Santo the edge on the national stage.
You've made some very good points, (info, which was all true.) That said, I think I may have to agree with you on this. That Trafficante was more powerful overall, than Marcello was.
Yes, Carlos Marcello was extremely powerful. (and yes, its true that he alone largely controlled the entire state of Louisiana. Whereas, Trafficante allowed all families to operate in South Florida which Cosa Nostra considered "open territory")
But, although the New Orleans "Family" was largely recognized as the first borgata on U.S. soil, and was given special status because of that, and Marcello supposedly held an iron first over LA politics and government officials, the Family, generally speaking, still largely operated as a local entity. I'm not aware of he or his men operating nationally, much less, across the globe.
On the other hand, (as you pointed out) Trafficante operated a much more wide-ranging Family, with very diversified criminal interests across the globe.
He was also the son, and successor, to Santo Trafficante Sr., who was himself one of the very first bosses, and an "original" from Sicily.
I also think that at the height of their respective power, the Tampa Family was larger than the New Orleans Family numerically.
In many ways, this is like splitting hairs between them, because they were both major powers, who, collectively, largely controlled the organized criminal underworld across the entire "Southeastern United States."