Carvajal, dubbed "El Pollo" (The Chicken), was taken into custody at his son's home by Spanish police.
Carvajal has long been sought by US Treasury officials who suspect him of providing support to drug trafficking by Colombian FARC guerrillas.
In May 2013, a Florida court accused him of having worked for Colombian drug traffickers from 2004 to 2010.
Carvajal was the highest-ranking army official to declare his support for Guaido, saying that the six years Nicolas Maduro's presidency had been a disaster.
On February 21, he posted a video on Twitter in which he told army officers: "How it all ends will depend on you my brothers in arms" and urging them to stand "on the right side of history".
Maduro then ousted Carvajal and he was accused of "acts of treason".
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