The man, who was charged with narcotics possession, was among 17 men held at Beetham Gardens between 5 a.m. and 9 a.m.
Police said the gang leader was initially targeted for detention last week following a spate of murders in east Port of Spain but he escaped the police dragnet during which 12 other gang leaders were held.
Two of the youngest murder victims — Nyam Antoine, 17, and his cousin Rasheeda Gomez,16 — were laid to rest earlier this week.
Police said the exercise yesterday began around 4 a.m. and involved 200 police officers and 50 soldiers led by Snr Supt Wayne Boyd along with ASP Ajith Persad and Insp Sahadeo Singh.
Officers said they sought out men who had outstanding warrants.
Three of the suspects were charged with narcotics possession, two were charged with selling alcoholic beverages without a licence while the remaining 17, including the gang leader, are to be interviewed by officers of the Criminal Gang Intelligence Unit.