The petition, started in late February, reached over 4.16 million signatures on Saturday and has the highest rate of sign-ups on record, according to the official Petitions Committee.
The second most popular is a 2016 petition calling for a second EU referendum if the Remain or Leave vote was less than 60 per cent, which gathered just over 4.15 million signatures.
In third place is a petition to prevent Donald Trump from making a state visit to the UK, with nearly 1.9 million signatures.
By contrast, the most popular pro-Brexit petition on the Parliament website which calls on the government to “leave the EU without a deal in March 2019” had received almost 460,000 signatures by Saturday morning.
The petition to revoke Article 50 has crashed several times since the petition leapt in popularity on Wednesday following Theresa May’s appeal to the British people to support her as she demanded MPs back her deal.
At one point nearly 2,000 people were signing up every minute. And signatures continued to be added even after the threat of a no-deal exit on 29 March was removed when EU leaders agreed Brexit could be delayed.
The constituencies with the highest number of sign-ups are Bristol West, Hornsey and Wood Green in London and Brighton Pavilion.
A number of MPs and celebrities have publicly backing the appeal, including Jennifer Saunders, Hugh Grant and Brian Cox.
When asked about the growing number of signatories on Thursday, Ms May said she did not believe in halting the deadline after the EU offered a delay plan.
As the petition attracted attention, conspiracy theories arose suggesting that a small proportion of signatures from addresses listed as overseas meant that the petition had been “hijacked by bots”.
But in a tweet, the House of Commons petitions committee clarified that 96 per cent of the signatures are listed as from the UK.
They added that overseas signatures were valid, since “anyone who is a UK resident or a British citizen can sign a petition. This includes British citizens living overseas.”
Analysis by software firm Tableau of the 16,000 petitions running on the government website showed the revoke Article 50 petition had more than three times as many signatures as all the pro-Brexit petitions combined.
Organiser Margaret Anne Georgiadou wrote: “The government repeatedly claims exiting the EU is ‘the will of the people’.
“We need to put a stop to this claim by proving the strength of public support now for remaining in the EU. A People’s Vote may not happen – so vote now.”
She added: “I do not believe that we should be revoking Article 50.”