More than 175 foreign criminals have been deported under a new crackdown, including a violent sex offender and an Indian man who attempted to defraud department store Harrods.
A further 314 foreign criminals were detained as a result of Operation Nexus, a joint initiative launched by the UK Border Agency (UKBA) and the Metropolitan Police Service at the start of September, the Home Office said.
The operation saw UKBA officers posted in 21 custody suites across London, allowing them to run real-time immigration checks on individuals brought into custody.
The figures came as the Home Office battles to deport radical preacher Abu Qatada to Jordan, where he was convicted of terror charges in his absence in 1999.
The Government is fighting against the decision of the Special Immigration Appeals Commission (Siac) to uphold Qatada's appeal against eviction.
Among the criminals removed from the UK under Nexus were Indian national Manindhar Annamdevula, 24, who was arrested for attempted fraud at Harrods in October, some five months after his visa had expired.
Shahnoza Sayfieva, 35, from Uzbekistan, was arrested in October on suspicion of blackmail and soon deported, while Ugandan Julius Amet, 36, was arrested in October for a public order offence and later deported.
Metropolitan Police assistant commissioner Mark Rowley said: "Nexus is not about targeting communities but making sure that, by maximising intelligence and smarter ways of working with UKBA and other international partners, we are as effective in dealing with offenders who are foreign nationals as we are with those from the UK."
Some 28% of all those arrested for a criminal offence in London are foreign nationals, recent Met intelligence showed.
Nexus combines police and immigration intelligence to tackle foreign criminals in London and has led to the removal of some of the capital's highest-harm criminals.
The operation also saw unknown fingerprints and DNA at police crime scenes being run against UKBA databases in a bid to solve previously unsolved crimes.
It also saw working relationships set up with police officers from countries where high volumes of offenders are identified, such as 20 officers seconded from Romania.