Character: Croc, while Doflamingo may have a fleshed out backstory, I didn’t like the direction Oda took with him in Dressrosa.
Design: this one is tough, they’re both really good. I feel like Doflamingo may be the more unique of the two, but Croc is essentially Captain Hook if he were a mob boss, so will go with him.
Powers: again, both are great. Unfortunately though, Doflamingo’s powers kind of got worse the further we got into Dressrosa, I wish we had gotten to see him Parasite a SH to fight the others and more stuff like Spider’s Web instead of Awakening, while Crocodile’s powers have remained fairly consistent, so giving it to Croc again.
Evil factor: oh boy, this is an awkward one. Doflamingo had some very dark evil moments, like when he took his father’s head back to Mariejois to try and get his World Noble status back, nearly drowning that gladiator while telling him that blood and death were “entertainment” for humans, tried getting Law to perform the fatal immortality surgery, and frequently used his powers to make people fight each other. On the other hand (hope this makes sense), his evil seemed forced/eyeroll worthy towards the climax of his arc, like how he kept ranting he had the blood of the gods, people were meant to be controlled by him, etc. It was just so awkward. Croc was no slouch either, tricking Alabasta into a civil war where many people died, all for the sake of acquiring a WMD and creating his utopia, and often passed the time sending a sandstorm purely to torture an old man digging for water, cruelly shutting down Vivi’s attempts to save her people, etc. I’ll give it to Doflamingo for this one, but I felt like his evil got too cheesy during the climax of Dressrosa.
Threat level: Crocodile by far, while it doesn’t help Dressrosa had Fujitora and Sabo there, Doflamingo made too many stupid decisions and got turned into a Saturday morning cartoon villain at the end.
Tl;dr, imo Doflamingo had the potential to be one of the best villains/characters, but while he certainly had some moments, Oda didn’t manage to do him justice. Crocodile was more consistent and lived up to his hype more, so I’d say that Crocodile > Doflamingo overall.