Mayor Boris Johnson has said he wanted London to become "a wi-fi city", where the internet was available anywhere.
"Let's do it, beginning in Stratford in this fantastic area of opportunity," he told BBC London 94.9, referring to the location of the main 2012 Olympic site.
He said this was better than a £300m plan announced by Gordon Brown, where vouchers for computers will be given to schoolchildren to get them online.
That sounded "a bit like a desperate bribe by the prime minister", he added.
Mr Brown used his main Labour conference speech to offer free computer access to children from low-income families, to boost their chances in the jobs market.
He said the 1.4 million youngsters without internet access lost out in the education needed to get good jobs.
Up to £700 in computer vouchers will be given to schoolchildren who cannot afford internet access.
"I certainly think there is a case for dealing with people who are information technology-poor, and trying to help people get online," Mr Johnson said.
"[But] what we need is a city where anywhere you go, you can log on, you can get on the web.
"They've done it in other parts of the world; why on earth can't we do it?
"I think that's the way we should be going, rather than bunging money to people, which sounds a bit like a desperate bribe by the prime minister," he added.
"Let's look at ways that we can improve the infrastructure in this city so that there's wi-fi access everywhere."
The mayor reiterated that Londoners would not face further increases in their council tax bills to fund the 2012 Games, and that the event would not exceed its £9.3 billion budget.
And he said that while London's Olympics would be "fantastic", organisers would not seek to copy some of the spectacular elements of Beijing's Games last month.
"Let me tell you what the International Olympic Committee said to me - all these distinguished Belgian lawyers and Swiss rowers.
"What they said is: 'Listen, Boris. This is London's Games. We know that it's going to be absolutely fantastic in London, but don't think you have to imitate the Chinese exactly. It's not possible and indeed it's not desirable, frankly.'
"What I think people want in a London Games is something that's more exciting, in a way, for the spectator.
"We can try and we are going to do better [than Beijing] but we're going to do it in our own sweet, distinguished, brilliant, ingenious British way."
Mr Johnson added there was a need to generate a "sense of excitement in the middle of the city", which he felt had happened in Sydney in 2000 but not in Beijing.
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