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A 33-year-old woman and a 32-year-old man - both pulled from the second-floor apartment where the blaze started - died. The man was identified as Tony Wang. The woman's name was not immediately released.
Authorities say Wang's apartment was right above the apartment where the fire appeared to start.
At least one other person was listed in extremely critical condition.
Emergency responders were met with a deluge of victims as they arrived at the scene.
Twenty residents and eight firefighters were hurt. Four of the residents were being treated for critical injuries.
One, a 57-year-old woman, apparently jumped from the building. She was rushed to Bellevue Hospital in unknown condition.
Other residents with less serious injuries stood on the fire escapes to get away from the flames.
The injured were taken to several hospitals, including Bellevue and New York University Downtown Hospital.
Assemly Speaker Sheldon Silver, who is from this district, released the following statement:
"The tragic fire this morning at 22 James Street has claimed the life of at least one person and injured several residents and firefighters and is devastating to me and my community. Although the blaze has badly damaged the building, I was relieved to know that firefighters and emergency services workers were able to evacuate so many residents from the building and nearby structures. Their task has certainly been complicated by the freezing weather. I salute the Red Cross workers who are near the scene to assist families in need of shelter. We have staff on hand to give assistance to those who have been displaced. At this time my thoughts are with the families of the deceased and injured residents, those displaced by this awful fire and the first responders who are so ably dealing with it."
Meanwhile, 60 families, estimated at more than 200 people, were evacuated.
"People were yelling and screaming from the fire escape. They were crying for help," Mary Liu, 29, told the New York Daily News. "One lady jumped out of the building. It was chaos."
Fire officials said three people jumped from windows, but all of them survived.
The fire, which started on the second floor, was difficult to control because the building was so old, like so many in the historic lower Manhattan neighborhood, McNally said.
Last month, a Buildings Department inspection found "defective/exposed" electrical wiring in ceiling fixtures throughout the building and violations were served, according to city records.
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