The search was launched when a neighbour called 112 to report seeing a man with blood on him chasing after his wife.
Police patrol cars went to the property and questioned the couple – who are parents of two young children aged around four and two years old – and took them both into custody.
They then launched a hunt of nearby areas to find the children. Local newspaper Las Provincias reported that blood had been found during the search.
Sniffer dogs were deployed in the search.