He took part in anarchist insurrections that marked the first years of the Republic, and in 1932 was detained and deported in Bata, on the coast of Río Muni, and then to the Canary Islands.
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With Carlo Rosselli, Berneri organized the first column of Italian volunteers to fight in the Spanish Civil War against Francisco Franco's attempted coup, where he took part in the battles of Monte Pelado and Huesca (in Aragon) together with the Spanish anarchists of Francisco Ascaso Column and the Italians of the Matteotti Battalion.
After that, and pressured by the Primo de Rivera dictatorship, Buenaventura Durruti, Francisco Ascaso and other members fled to France, and then to Latin America, where they were charged with more robberies.
Resenting the violence with which trade unions were met by employers, he formed the anarchist group Los Solidarios, together with Buenaventura Durruti, Francisco Ascaso, Juan García Oliver, Gregorio Jover, Ramona Berri, Eusebio Brau, Manuel Campos, and Aurelio Fernández.