A method and apparatus for removing pollutants from organic solid waste by pyrolysis coupled with chemical looping combustion are provided. The apparatus includes: an air reactor, a fuel reactor, and a pyrolysis gasifier. The pyrolysis gasifier is sleeved outside the fuel reactor, and the air reactor is connected with the fuel reactor. A top end of the air reactor is connected with a top delivery pipe; the top delivery pipe is connected with a first cyclone separator; and the first cyclone separator is connected with an oxygen carrier refeeder provided at a top end of the fuel reactor. The apparatus forms a two-stage reaction unit of pyrolysis and chemical looping combustion by decoupling the pyrolysis process from the chemical looping combustion, which avoids the contact between the complex ash of organic solid waste and the oxygen carrier, thereby improving the service life of the oxygen carrier.