Mayor of London Sadiq Khan wants TfL to take immediate control of Southern Rail in a bid to end months of misery for thousands of commuters.
The TfL team would run Southern Rail until the government is able to resolve the longer-term problems that have he has described as "an embarrassment to our city".
And now, in a letter to Mr Grayling, the mayor of London has slammed the department's failure to resolve the ongoing train chaos.
He said: "Thousands of Londoners and longer-distance commuters simply cannot get to and from work, and are understandably furious.
"There is no doubt that the franchise must now be in default, and I have previously called for your department to step in and take control.
"Notwithstanding the wider discussions on devolution, I now offer to go one step further and put my senior TfL team in charge of the GTR Southern franchise until we get a permanent resolution."
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After months of delays and cancellations, Govia Thameslink Railway Southern franchise brought in an emergency timetable which scrapped 341 services.
But this left commuters crammed onto packed trains or stranded on replacement buses.
Len Duvall, the London Assembly Member for Greenwich and Lewisham, said:
"Of course this is the right step to take.
"When passengers are paying out a lot of money in fares, it’s anger-inducing that they are receiving such a poor service.
"Government’s weak approach to tackling Southern over their staffing issues and sub-standard performance has left passengers in purgatory.
"A TfL takeover is a sensible step towards addressing the problems plaguing Southern, which the government have so far been content to kick into the long grass."
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