Protesters had occupied the site to express their concerns about new artistic director Chris Dercon, the former head of London's Tate Modern, whom they fear will lead the radical theatre towards a more commercial direction.
The protest at the building in east Berlin began on Friday and by the weekend, the crowd had swelled to the theatre's maximum capacity of 500.
Berlin police on Thursday deployed 200 officers to clear the space.
"There are now no longer any unauthorised people in the Volksbühne. We accompanied 21 people out of there, five of them were carried out," police said on Twitter.
Volksbühne artists have been strongly critical of Dercon, who replaced the renowned Frank Castorf who led the avant-garde theatre for almost a quarter of a century.
Rebuilt after World War II in an imposing Stalinist style using remnants of Hitler's destroyed chancellery, the Volksbühne prides itself on caustic commentary on political and capitalist hypocrisy.
A prominent theatre director as well as artistic director, Castorf was credited with turning the Volksbühne into one of Europe's leading venues with his bold, controversial and often lengthy productions.
Dercon, whose nomination has been controversial ever since it was announced in 2015, will be the first non-artist to take the helm of the fabled theatre.
Critics fear his tenure will herald a shift to less provocative and more commercial productions at the heavily subsidised Volksbühne.
They have also questioned whether Belgium-born Dercon can bring the radical sensibility and awareness of Berlin's tumultuous history that is woven into the fabric of the theatre.