Hunted by security forces across the Caribbean island, Christopher "Dudus" Coke sought out a preacher's advice and tried to turn himself in to US marshals but was caught by police at a highway checkpoint before he could get there.
Police Commissioner Owen Ellington urged Coke's gangland supporters to allow the law to take its course.
Last month, 76 people were killed in fighting between security forces and gunmen loyal to the man branded by US authorities as one of the world's most dangerous drug lords.
"I would like to appeal to the families, friends and sympathisers of Christopher Coke to remain calm," Mr Ellington said after the capture of Jamaica's number one fugitive, who eluded the bloody police offensive in his West Kingston slum stronghold.
Security forces "are taking every step possible to ensure his safety and well-being while he is in our custody", Mr Ellington said, adding that legal proceedings against Coke should get under way quickly.
The 42-year-old Coke, who faces trial in New York on drug-trafficking and gun-running charges, is said to fear suffering the same fate as his father, a gang leader who died in a prison fire in 1992 while awaiting extradition to the US on drug charges.
Mr Ellington said Coke was caught by police manning a vehicle checkpoint along a highway, but added that other "circumstances of (Coke's) arrest are being investigated". He said police were acting on intelligence.
The Rev Al Miller, an influential evangelical preacher who facilitated the surrender of Coke's brother earlier this month, told The Associated Press that Coke was heading to surrender to authorities at the US Embassy in Kingston when police stopped his convoy on a highway outside the capital.
"A contact was made on his behalf that he wanted to give himself in," Mr Miller said. "I therefore made arrangements with his lawyers because he wanted to go ahead with the extradition process, so we communicated with the US Embassy because that's where he would feel more comfortable."
Mr Miller said police took Coke to the nearby Spanish Town police headquarters, then flew him to Kingston.
Last month, a US law enforcement official in New York, speaking on condition of anonymity, told the AP that a lawyer for Coke was negotiating with the Justice Department about his client's possible safe removal to New York to face charges.
A phone listed for Coke's lead lawyer, Don Foote, went unanswered.
Preet Bharara, the US Attorney for the Southern District of New York, said, "We look forward to working closely with the Jamaican authorities to bring Coke to justice to face charges pending against him in Manhattan federal court."
Coke is wanted in New York on charges that he trafficked cocaine and marijuana as well as weapons between Jamaica and the United States. Coke, who typically avoids the limelight, faces life in prison if convicted.
Prime Minister Bruce Golding, whose Jamaica Labour Party has long counted on the support of gunmen inside Coke's stronghold in the Tivoli Gardens slum, opposed the US extradition request for nine months before doing a U-turn under growing public pressure that threatened his political career. His stand also strained relations with the US.
Earlier this month, the main opposition party staged a no-confidence vote against Mr Golding, which he survived after promising a sustained assault on the gangs which control poor politicised slums like Tivoli Gardens.
Jamaica's political history is intertwined with slum gangs that the two main parties helped organise - and some say armed - in Kingston's poor neighbourhoods in the 1970s and '80s. The gangs controlled the streets and intimidated voters at election time. In recent years political violence has waned, and many of the killings in Kingston now are blamed on the drug and extortion trade.
Coke was born into Jamaica's gangland. His father, known as Jim Brown, was the leader of the notorious Shower Posse, a cocaine-trafficking gang with members in Jamaica and the US that began operating in the 1980s and was named for its members' tendency to spray victims with bullets. The son took over from the father, US authorities allege.
Hours before Coke's arrest, Jamaica's government extended a month-long state of emergency to St Catherine parish, where he was captured.
Mr Golding has pledged to crush street gangs and replace their strong-armed rule with social programmes for the poor. But the vow has a hollow ring in the gritty slums where "dons" like Coke have long provided services and imposed a disciplined law and order the government could never achieve. Slum dwellers have a deep distrust of the police, who are often seen as agents of the country's elite.