1) Willie Marfeo: not really a gangster, just an illegal bookmaker. I like him because, when extorted for money, he had the balls to give Tameleo a slap on the face calling him an asshole, and told him to tell Patriarca to sh#t in his hat. In the 60s that was a 100% death sentence, therefore it was a stupid action not to go into hiding after this, yet it's impressive nevertheless, imo.
2) Carlo Caputo (boss of the Madison family): never really bothered anyone, no massacres or high-profiled murders on his turf, just quietly stayed at home without paying taxes.