Deaths related to drug poisoning was the leading cause of death in England and Wales, too, although making up less of a proportion of deaths at almost two-fifths.
ONS also found an estimated 99 suicide deaths and 71 alcohol-specific deaths, accounting for 13 per cent and almost 10 per cent of deaths in total.
Covid was involved in only 3.5 per cent of cases registered in 2021.
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Most deaths were recorded in London and the north-west of England, making up 20 per cent and 15 per cent of deaths respectively.
The majority of people who died were men, who made up 87 per cent of all deaths, and the most common age of death was between 45 and 59 years. Women were more likely to die at a younger age than men with a quarter of all female deaths between 40 and 44 years of age.
There was a sharp increase in the number of young people who died while homeless. An estimated 31 people aged between 16 and 24 years old lost their lives without a stable home, representing a 63 per cent increase on 2020.
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Charity Centrepoint’s director of policy Balbir Kaur Chatrik said: “Any death as a result of homelessness is unacceptable. But there is something especially heart-breaking to hear that the number of deaths among young people has increased.
“These young people had so much of their lives ahead of them, they deserve more – they deserve a chance to turn their lives around, but they can’t do this if the right support isn’t there.”
Homeless Link chief executive Rick Henderson described the figures as “shameful”. The charity’s recent report into health inequalities found more than three-quarters of people experiencing homelessness were living with a physical health condition while 82 per cent reported a mental health diagnosis.
“We should not and cannot accept poorer health outcomes for people experiencing homelessness. These ONS stats are damning indictment of what happens if we do,” said Henderson.
A government spokesperson said: “Good progress has been made towards tackling rough sleeping with the number of people sleeping rough down 49 per cent since 2017. But we also know how tough many people are finding things in the current economic climate
“These statistics are another reminder that there is still much more to be done. Our goal remains to keep people off the streets in the first place and to get those on the streets the help they need. We are providing £2billion over the next three years to tackle homelessness.”
The ONS uses a similar method to counting homeless deaths as the National Records of Scotland.
Statisticians search death registration records to find evidence that people died while homeless and use modelling to estimate the likely number of additional deaths not picked up in searches.
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James Tucker, data and analysis for social care and health at ONS, said: “The latest figure is more in line with pre-pandemic levels following a notable fall in 2020, although it’s too early to say whether this is a resumption of an upward trend in homeless deaths.
“Any death in these circumstances is a tragedy and our estimates are designed to help inform the work of everyone seeking to protect this highly vulnerable section of our community.”
That method differs from the Museum of Homelessness’s (MOH) approach in its official Dying Homeless count.
MOH uses freedom of information requests and submissions from members of the public to produce its UK-wide annual count.