The 20-year-old, who starts Cambridge University next month to read history, poses for a shoot inspired by French musician Serge Gainsbourg's Melody Nelson album.
It shows the Marks and Spencer model holding a teddy bear, wearing nothing but a pair of white socks on the cover, with a further 14 pages of pictures inside.
French Playboy's fashion director Alex Aikiu told the Daily Mail the model did not ask for a large fee for the shoot.
He said: "It's all about being sweet and innocent.
"We just paid her the editorial fee any magazine would. Lily said yes right away."
When speaking of Cole's interview, Mr Aikiu added: "It's very intimate, very psychological. For us, Playboy isn't Pamela Anderson. It doesn't matter how big your boobs are - it's about what's inside the woman."
Cole recently admitted she cannot wait to start university.
She said: "I'll still do bits of modelling alongside my degree. We have long holidays, so I'm hoping I'll be able to work then.
"But modelling can get a little lonely sometimes, especially when you are travelling on your own. That's what I'm looking forward to about going to university to meet lots of new people."
Gainsbourg is probably best remembered for his worldwide hit "Je t'aime... moi non plus", a duet with his lover Jane Birkin.
source: telegraph.co.uk
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