Redbridge Council has been awarded £625,000 from the government to help end rough sleeping.
The grant is part of the government's £112million fund to help get people off the streets and into accommodation.
Last year saw a reduction in the number of rough sleepers in the borough, the council said.
But new figures from the Combined Homelessness and Information Network (Chain), which is commissioned and funded by the mayor of London, shows that Redbridge had the highest number of rough sleepers among outer London boroughs between October and December last year.
Across the boroughs, there were 1,169 recorded during this period, an increase of 382 from the previous year.
Of these, 112 were in Redbridge. Between October and December 2018 there were 28 rough sleepers in the borough.
In 2019, this jumped to 77 between January and March, 95 between April and June and 92 between July and September.
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Overall, the data reveals that 3,637 people slept rough across the capital from October to December last year, an 11pc increase from the same period last year.
In the past year, Redbridge Council has opened a second homeless shelter, invested in the Housing First specialist supported housing service, and helped rough sleepers find employment.
The council will also shortly be opening Project Malachi in Ilford, a temporary housing scheme, created in partnership with the Salvation Army.
It will provide 42 flats with on-site support for people who were previously homeless and sleeping rough.
The council said it will use the government funds to expand the care and resettlement support for the most vulnerable rough sleepers, and expand the Housing First specialist supported housing.
Councillor Farah Hussain, cabinet member for housing and homelessness, said: "The award acknowledges that unfortunately more and more people are becoming homeless in Redbridge.
"This money will make a huge difference to these people's lives, although we could obviously do more with additional funding.
"There are many reasons why people become homeless and sleep on the streets, and we will continue to work tirelessly with our partners to support them into secure accommodation. These are some of the most vulnerable people in our society. We are determined to put an end to rough sleeping in our borough."