He said the government "has been seriously complacent about this health emergency for the last six years and now is the time for them to stop gambling with our health and show real leadership".
Following the high court ruling (in which the Mayor was an interested party), saying the government had broken the law by failing to tackle illegal levels of air pollution, the London Mayor wants a fresh package of measures introduced as soon as possible.
He's currently consulting on measures including a new T-charge in the congestion charging zone from next year, as well as introducing the ultra low emission zone a year earlier in 2019.
But Khan said: "After years of failure we now need the government to get a grip and face up to their responsibilities rather than pass the buck to me and boroughs. Let's be clear, filthy air is causing 9,400 deaths every year in London alone. And that's before you look at all the other health problems caused to Londoners."
Khan wants a national diesel scrappage scheme and a Clean Air Act "fit for the 21st century".
The government's plans for tackling the UK's air pollution troubles were judged illegally poor at the high court - the second time in 18 months that ministers have lost in court on the issue. Legal non-governmental organisation ClientEarth brought the case, arguing that current plans ignore many measures that could help cut the levels of nitrogen dioxide in the shortest possible time.
The government agreed in court to discuss with ClientEarth a new timetable for more realistic pollution modelling and the steps to take to bring pollution down to legal levels.
Theresa May said at prime minister's questions: "Nobody in this house doubts the importance of the issue of air quality. We have taken action, there is more to do and we will do it."
The capital's black cab drivers are holding a protest on Tuesday to call on the government to tackle traffic congestion and pollution in the capital. They're expected to bring Whitehall to a standstill at 2pm.