The incident happened at about 3:30 p.m. on Decatur Street in the Bedford Stuyvesant section.
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Law enforcement sources said one of the four men came up behind the 99-year-old woman, threw a blanket over her head, and tied her up. The robbers then tied up her 91-year-old husband.
The men then tore through the couple's home, stealing various items.
Photos: Scene of deadly home invasion in Brooklyn
Police said the woman was able to break free at some point and call 911. Officers rushed to the home, but the robbers were gone.
The man suffered some sort of injuries during the ordeal and was rushed to the hospital where he died a short time later. His wife was being treated by paramedics at the scene.
"It was like a loud boom," a neighbor who heard the commotion said. "I thought it was a gunshot initially. That's what I thought it was. But it wasn't a gunshot. From in the neighborhood, they're basically saying they were robbed and the gentleman had a heart attack."
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NYPD detectives are searching for the four men who were involved in the deadly home invasion.