The 49-year-old, who has not been named, is thought to be behind 15 hold-ups in the provinces of Malaga and Alicante, accompanied by a 31-year-old Russian woman.
Spanish police believe the pair could have stolen about 115,000 euros (£98,345) in the raids.
They are suspected of working together to carry out the crimes, a police spokesman said.
Detectives believe their modus operandi involved the woman first ringing the bell of the bank and when a member of staff opened the door she would be flanked by the man, who was armed with a pistol.
He would then enter and rob the bank.
In some cases the man threatened staff by holding the pistol to their heads, detectives said.
When the pair were arrested, officers seized a car, a pistol, a laptop case, two wigs, a fake beard and moustache and a purse containing stolen money.
Officers from Spain's Civil Guard swooped following a five-month investigation beginning in mid-April and codenamed Operation Flanders.
The probe was launched after a bank robbery in the Malaga town of Mijas on April 16.
This was followed by another one in the Alfaz del Pi area of Alicante.
The man and woman arrested are believed to have been responsible for both.
In the following months they are suspected of committing another five robberies in the areas of Calpe, Alicante, and the Malaga resorts of Sabinillas, Cala de Moral and Torrox.
A police spokesman said: "During the investigation the Civil Guard became aware that previously, from 2008, the suspects had committed three other robberies in (the Costa del Sol resort of) Fuengirola and five more in Marbella."
The last robbery was committed last Friday at 9am local time in the Torrox area.
After being alerted to the incident, the Civil Guard and Judicial Police set up vehicle control points in order to intercept the suspects.
Officers were deployed to different locations around the Mijas and Marbella areas of Malaga.
At about 10am, a group of Civil Guard officers stationed near a toll barrier on the A7 motorway saw a car that matched the description of that used in the robbery.
When they recognised the people inside it, they stopped the car and arrested them, a spokesman said.
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