A series of so-called Baileys Chilled Sundays screenings will run from the end of this month until Christmas, at cinemas in Clapham, Greenwich, Brixton and Stratford.
Filmgoers will be able to pay £3 to watch classic movies including Breakfast at Tiffany's, Amelie and Love Actually, with the price including a free sample of Baileys. The deal was negotiated by the company's media agency, Carat, with films running from 4pm to 6pm.
Baileys' previous involvement with cinema involved sponsoring exclusive previews of the film Intolerable Cruelty. A CSA spokesman said: "It's good to welcome a sponsor like this back to cinema."
Other films lined up for the Carlton/Baileys sponsorship include Strictly Ballroom, Top Gun and Gladiator, appealing to movie fans of different ages.