The site for the News International-owned tabloid achieved 27.3 million unique users for the month of February, up from 21.9 million unique users in January. It also achieved the biggest annual increase in the sector, up 118% year on year.
In stark contrast, February proved to be a difficult month for Guardian.co.uk, which followed its record-breaking January figure of just below 30 million with a dramatic 15% drop to 25.3 million unique users.
It marks the first time the Guardian website has not led the field since May 2008, when it was overtaken by The Daily Telegraph and the Daily Mail.
Emily Bell, director of digital content at Guardian News and Media, welcomed the competition and stressed the site continued to attract the biggest UK-only audience.
She suggested a weaker international news agenda may have had an impact on January's Obama-driven performance and added: "By contrast, the celebrity agenda was very active and this may account for the overall increase in some of our competitors' figures."
February's third-most popular national newspaper website, Times Online, reported a near-4% drop in figures from 22.9 million unique users in January to 21.9 million in February. It just remains ahead of the Mail Online, which reported a 5.2% drop in figures from January to 21.8 million unique users.
The Independent also reported a decline in users, dropping 8.4%, from 10.2 million to 9.3 million unique users.
The Telegraph reported a small 1% increase from January to February, from 25.9 million unique users to 26.1 million.
Trinity Mirror-owned site Mirror Group Digital, which includes Mirror.co.uk increased its unique user base in the last month by 5% to 6.9 million unique users and increased by 83% year on year. More than 50% of the site's users are UK consumers, compared with 48% who access the site abroad.
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