Usually, he’s seen in memorable supporting roles with colorful names – two-bit thief Carl Showalter in “Fargo,” Donny Kerabatsos in “The Big Lebowski,” the hapless Seymour in “Ghost World,” Tony Blundetto in “The Sopranos.”

Sunday, he gets the biggest role of his career, portraying the Atlantic City kingpin Nucky Thompson in the lavish “Boardwalk Empire” on HBO.

“This is one of the best parts I’ve ever had in my life, and it’s just so exciting for me to go to work and to know that these scripts are so strong and to play a character who is ambitious,” Buscemi exuded during the TV Critics Press Tour in Los Angeles last month.

“He certainly has a dark side, but there’s certainly a lot of humor that goes along with it. I think he genuinely has a good heart and that he wants to share the wealth and help people. And he likes being a politician, and he likes being a leader.”

Givein the opportunities afforded by Prohibition, “you’re either on the trolley, or you can be put six feet under.” And Buscemi’s been enjoying his ride. “It’s so much fun to play a role like this. Really every day going to work was a pure joy.”

“I always wanted to work with Steve again,” says executive producer Martin Scorsese, who sets the tone for the series by directing the 75 minute premiere.  “I’ve been watching Steve’s work since ‘Parting Glances’ back in the ’80s, and we got to work together briefly in ‘New York Stories.’

“I love the range he has and his dramatic sense but also his sense of humor, and there’s something that’s very, very strong on the camera, with Steve as a character, whatever he plays, whether it’s in ‘The Big Lebowski’ or ‘Ghost World’ or any of these films.

“And I think it was a very interesting idea that Steve would play this part because it’s a character, as Steve says, that I do think basically is a decent guy, but in that world — it corrupts him so much. He’s a pragmatist, too. He’s practical. He’s put in the position of being a treasurer. Yet the treasurer runs the city in a sense, and ultimately, it’s the line towards the — in one of the episodes that you see which is, like, you make a deal. You figure out how much sin you can live with.”

Buscemi’s character isn’t just a tough gangster. He pauses at the storefront show of premature babies and looks into the fortune teller’s windows wondering what his future would be. And he spends a lot of time helping out an immigrant woman played by Kelly MacDonald. When he finds she’s in an abusive marriage, for example, Nucky has the husband killed – and blamed for a gangland murder.

“In a weird way,” Buscemi says, “It’s kind of true that he feels like he needs to save her, and it just so happens that his death could be very useful to what just went down, this big mistake that happened in the woods that shouldn’t have happened.”

But he adds, MacDonald’s character Margaret Schroeder “awakens something in him that he hadn’t felt since he was married, and his wife died about seven years before. But I think he genuinely likes people, and he, you know, the real guy, you just hear all the stories about him, about how he was so generous and really helped people out and wanted to see people prosper. I’m sure part of that was also getting reelected, but I have to believe that there’s something in him that wants to do good.

MacDonald looks at her character as someone willing to do what she has to in order to adapt. “She’s a survivor. You know, she emigrated to America with a view to get a better life for herself, and things don’t go quite as she had planned, but she’s okay with that. She’s married to a man who’s abusive and drinks their money away, but, you know, they’ve got children. That’s what she’s doing. That’s her life, and then when that all changes, she’s got a very strong survival instinct, I think. And she connects with Nucky’s character. She sees something in him. I think at the start, she sees something that isn’t quite there, you know, when he’s making a speech to the Temperance League, which is all just a big lie, but she connects with that story somehow, and that starts the series of events. But I think she sees something in him that other people may be doing, and she brings something out in him that is quite special.”

Buscemi is humbled, in the end, at what a big role this is for him.

“I mean, only in my wildest fantasies or dreams, you know, and when I first read the script, I could tell from page one that this was — you know, this was the man. And it was sort of terrifying in a way but also so exciting, you know. And when I first read the script, I hadn’t gotten the offer yet to play the character, and I just thought, wow, I’m almost sorry I’m reading this because, if I don’t get it, I’m going to be so disappointed, so sad. So, of course, when Terry did call me and he said that ‘Marty and I wanted’ me to play this role, my response was, ‘Terry, I know you’re looking at other actors, and I appreciate just that, you know my name is being thrown in.’ He says, ‘No, no, Steve. I just said we want you.’

It was quite a shock, he says. “It still didn’t sink in.”

Buscemi says he’s excited to be working once more with Terence Winter, with whom he worked on “The Sopranos,” and with Scorsese, who he calls ” the most energetic person on set, and it just inspired everybody. So just selfishly, I hope this continues for years and years.”

Could it? Writer Winter says, ‘Yes, certainly. I mean, the ’20s itself just as a backdrop — there’s so much material there, and I think the world we’ve created and the characters and how they relate and interact with each other, hopefully lends itself to a really long narrative. You know, it’s almost an epic novel, I would hope. And, you know, God willing, we’ll have the opportunity to do that.”

“Boardwalk Empire” starts Sunday at 9 p.m. on HBO.

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