The man, aged 49, and his wife, aged 53, were detained on suspicion of money laundering at their home near Guildford.
Around £15,000 cash was seized following searches of the property, along with items worth an estimated £150,000.
The pair are suspected of using airline staff to smuggle criminal cash and other high value items out of the UK via Heathrow Airport.
They remain in custody and are being questioned by NCA investigators.
