The charges against the three Moroccans and one Spaniard came after hours of questioning at the National Court, and bring to nine the number of people charged in the March 11 railway bombings.
The charges stop short of a formal indictment, but suggest the court has strong evidence against the suspects. They will remain in jail while investigators gather more evidence.
A fifth suspect, also Moroccan, was released without charges.
A total of 13 people are now in custody over the bombings, which left 202 people dead and more than 1,800 wounded. The latest four arrests came Monday in Madrid.
Spaniard Jose Emilio Suarez, accused of providing explosives for the attacks, was charged with 190 counts of murder, 1,430 counts of attempted murder, robbery and collaborating or belonging to a terrorist organization. Court officials said the latter charge will be specified further as the probe continues. The figure of 190 cited by the judge is the number of bodies officially identified so far.
Moroccan Abderrahim Zbakh was charged with all those same offenses except robbery.
Mohamed El Hadi Chedadi and Abdelouahid Berrak, also Moroccans, were charged with collaborating with or belonging to a terrorist organization.
The freed suspect was named as Farid Oulad Ali. Judge Juan del Olmo said there was insufficient evidence against him.
Chedadi, the brother of a suspect jailed in Spain in 2001 on charges of being part of a Spain-based cell that allegedly helped plan the Sept. 11 attacks in the United States, denied any involvement in the Madrid attacks and said he learned of them that same morning while watching cartoons at home with his children, court officials said.
The Spaniard, a former miner, admitted helping Moroccans still at large obtain explosives but said he did not know what the dynamite would be used for.