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Fernando Medina estimated that more than a third of properties in the centre of the city are currently taken up by holiday lettings.
Writing in The Independent, Mr Medina said tourist rentals had pushed up property prices in recent years and driven out essential workers and their families.
To tackle the problem, authorities will offer to pay landlords in return for renting "safe homes" as affordable housing for workers including hospital staff and teachers.
As well as the rental initiative, authorities hope to create more cycle lanes and parks as part of the city's green recovery following the coronavirus pandemic.
"Now we want to bring the people who are Lisbon’s lifeblood back to the centre of the city as we make it greener, more sustainable and ultimately, a better place to both live and visit," Mr Medina wrote.
The mayor cited examples of other cities that were also implementing "bold" strategies to change their urban spaces for the better.
He wrote: "From Melbourne to Paris, the tide is turning against urban sprawl and back to revitalised city centres where residents can reach key services, like doctors, schools and shops all within a 20-minute walk."
He added: "With many more people likely to be permanently working from home, it makes sense for more Lisboetas to swap the suburbs for the city where they can easily access public transport, services and take advantage of festivals and concerts."
The impact of rental platforms such as Airbnb has come under growing scutiny in cities around the world.
Earlier this year, the French government announced its plan to create a state-run booking website in an attempt to rival websites such as Airbnb and Booking.com as the county tries to revive its tourism sector in the wake of the coronavirus pandemic.
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