Ban private cars in cities. Seriously.
I love the idea, but people would doubtless claim it was an infringement of personal liberties. However, doing what London has done, charging people a high fee to access central areas, may not a bad starting point. People with disabilities, special circumstances etc., could apply for dispensation, or reduced costs. If all it does is hurt people who can't afford it, it's not a win, but it may be better than what we have.