Scotland Yard says there has been a five-fold increase in UK nationals travelling to Syria or Iraq for terrorism purposes.
Police said 69 suspected extremists have been arrested so far this year who planned to travel to Syria or fund terrorism there.
Assistant Chief Constable Mark Rowley, of the Metropolitan Police, appealed to family members of potential UK terrorists to come forward and said nearly half of would-be extremists identified as part of the Syria investigations were not previously classed as dangerous.
He said: "The biggest growth in Syrian-related investigations has occurred in London and the West Midlands.
"The growth of dangerous individuals poses challenges for policing, especially when nearly half of Syria travellers of concern were not known as terrorist risks previously.
"Hence, we appeal to the public to help identify for us aspiring terrorists - they may be about to travel abroad, have just returned or be showing signs of becoming radicalised."
Mr Rowley added that seizures of cash which people had been trying to take out of the country to fund Syria-related terror activity have also doubled.
Investigators are attempting to get hundreds of piece of terror-related content linked to Syria removed from websites including YouTube, Facebook and Twitter.
Mr Rowley said police in the UK are trying to prevent hate crimes that could be influenced by events abroad, including anti-Semitic offences related to the Gaza conflict.
He added: "There is a lot at stake.
"In addition to the public assistance in identifying potential terrorists, we all need community and religious leaders to continue to speak out against warped narratives and we need everyone to ensure that public debate does not give oxygen to the terrorists by giving them the publicity they seek."
An estimated 500 Britons have travelled to Syria and Iraq to fight alongside extremists, half of whom are thought to be from London.
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