A Harlem man who was out on bail after previously being charged with trying to kill police officers during a shootout was charged on Tuesday with killing two men over Easter weekend, according to the New York Police Department.

The man, Messiah Nantwi, 21, of Harlem, was arrested on Tuesday and charged with murder for shooting each man in the head in two separate incidents, the police said.

He was also charged with one count of criminal possession of a weapon, the police said. Mr. Nantwi was expected to be arraigned in Manhattan, though the district attorney’s office could not confirm a time or date.

The police first responded at about 4:45 p.m. on Saturday to a 911 call reporting a man shot near the corner of Madison Avenue and East 132nd Street. The victim, who was 19, was brought to NYC Health and Hospitals/Harlem where he was pronounced dead. The police have not identified him.

Then, just before 8 p.m. on Sunday, officers responded to a 911 call about a man shot inside a smoke shop on Malcolm X Boulevard near West 125th Street in Harlem.

They found the victim, Brandon Brunson, 36, of East New York, Brooklyn, with a gunshot wound to the head, the police said. He was brought to NYC Health and Hospitals/Harlem where he was pronounced dead.

In 2021, Mr. Nantwi was charged in the Bronx with first- and second-degree attempted murder for shooting at a police sergeant and two police officers, according the indictment in that case.

Officers had spotted Mr. Nantwi and a second person on Feb. 21, 2021, carrying spray paint cans at Elton Avenue and East 153rd Street, prosecutors said at the time.

When officers tried to arrest Mr. Nantwi, he pulled out a .22-caliber pistol and fired three shots at the sergeant, Darren Earl, and the officers, Malik Underwood and Erick Reyes, according to the authorities.

The officers and the sergeant then fired 31 shots at Mr. Nantwi, striking him several times. He was treated at Lincoln Hospital, according to a March 2021 news release from the Bronx district attorney. The officers were not injured.

Mr. Nantwi was also charged at the time with criminal use and possession of a firearm, three counts of menacing a police officer, resisting arrest and possession of graffiti instruments, among other charges.

Patrice O’Shaughnessy, a spokeswoman for the Bronx district attorney, said Mr. Nantwi was jailed after his initial arraignment.

After a grand jury formally indicted him, a judge set a $300,000 bail. Mr. Nantwi posted 10 percent of that, $30,000, as bail laws permit, she said. He has been out of the custody of the city Correction Department and awaiting trial since mid-2021, Ms. O’Shaughnessy said.

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