The married actors have lived in Madrid for the majority of the relationship, but are reportedly looking to start a new life in London.
The Spanish couple, who tied the knot in 2010, are said to be seeking a quieter life for their expanding family (they welcomed a daughter, Luna, earlier this year).
Earlier this week, 39-year-old Penelope was spotted shopping in the English capitalamid rumours that she is looking for a home in the city.
The duo are said to have enjoyed living in London while 44-year-old Javier was filming for the latest James Bond film, Skyfall.
If Javier and Penelope do decide to make the move they will soon have to find a school for their three-year-old son Leonardo.
After Leonardo's birth in 2011 the couple swapped LA life to move back to their native Spain.
"This is not the place where I want to raise my children," said Penelope of her Hollywood home.
"When you have children, your attention is focused on the most important things," she added. "Now that I have children that keep me very busy, my priority is my family. Every day I appreciate the people that I have in my life more."
Penelope's thoughts on raising children in LA echo those of her fellow A-list actress, Gwyneth Paltrow.
"I don't want them [my children] to be teenagers in LA. No way," Gwyneth told Red magazine. "I'm looking at this like two years, three years tops, then we will go back [to the UK]."