London's Ultra Low Emission Zone (ULEZ) could be expanded to cover most of the capital by next year under new plans.
To date the ULEZ in central London has helped halve lethal nitrogen dioxide by the roadside, the mayor's office said.
Filthy air factored in about 4,000 premature deaths in 2019 - the greatest number in outer London, it said.
Data suggests the plan could deter more than 100,000 of the most polluting cars daily, but some MPs fear extra charges will worsen the cost of living crisis.
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3D map showing London air pollution in 2006
Transport for London (TfL) has started a consultation on expanding the ULEZ from 23 August next year, with the main aim of tackling toxic air quality.
The highest number of early deaths linked to poor air quality were in Bromley, Barnet, Havering and Croydon, and it is estimated harmful emissions could cost the NHS and social care £10.4bn over the next 30 years if no further action is taken, the mayor's office said.
Rosamund Adoo-Kissi-Debrah has campaigned on the issue since her daughter Ella became the first person in the UK to have air pollution listed as the cause of death on their death certificate in 2020.
She said: "Illegal levels of air pollution on the South Circular caused my daughter Ella's deadly asthma nine years ago [and] expanding ULEZ London-wide can help prevent future deaths like Ella's."
London Mayor Sadiq Khan said improving air quality was "the right thing to do" because "the air Londoners breathe is so toxic it stunts children's lungs, exacerbates chronic illness and contributes to thousands of premature deaths each year".
Alex Williams, TfL's director of city planning, said: "We must act at pace to tackle this, which is why we are proposing to expand the ULEZ London-wide next year and are looking at the longer-term solution of a new form of road user charging."
The plans have attracted criticism in the House of Commons.
Conservative MP for Harrow East, Bob Blackman, accused Mr Khan of "hammering hard-pressed motorists yet again".
Responding, Transport minister Andrew Stephenson said: "Decisions on road charging are of course for the Mayor of London alone to take, but I agree... the mayor must not punish people who need to use their cars, especially at a time when people are struggling with the cost of living."
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