Ascaso lived a life of crime and violence being involved in the deaths of multiple high-profile government officials and as a result frequently detained.

By the time of the Spanish Civil War, he had created and been involved in numerous anarchist operations and organizations alongside his close friend Buenaventura Durruti.

[2] In 1922 or 1923, Ascaso would meet Juan Garcia Oliver and Buenaventura Durruti, and soon form the Los Solidarios in response to the execution of the anarchist Francisco Ferrer.

[4] He would gather the funds of the Los Solidarios and travel to San Sebastián hoping to aid Durruti in achieving a pardon however this would not happen.

Ascaso and Oliver become embroiled in a conspiracy to assassinate then Archbishop of Zaragoza Juan Soldevila y Romero which they would successfully execute on 23 June 1923.

[4] In late December, 1924, Ascaso and Durruti were informed of the Revolutionary Committee's dire financial situation and so were instructed to travel to Latin America which they promptly did with the intention of collecting funds.

In late March 1925 Ascaso and Durruti were seeking refuge in Mexico City however soon left, feeling guilty over living in a luxury hotel juxtaposed to the poor neighborhoods.

[4] On 25 June 1926 Ascaso was arrested by French Police, sentenced to six months, with intent to harm the King of Spain who was visiting France at the time.

[6] An initiative entitled the Durruti-Ascaso-Jover Asylum Support Committee by The Anarcho-Communist Union was formed intending for the three men's release.

In January 1928 Ascaso and Durruti traveled to Paris for the purpose of meeting with Joaquín Cortés as well as anarchist groups of the time.

[1] Ascaso alongside Durruti and the CNT would attack army depots and the prison ship Uruguay with home-made grenades and improvised armoured cars.