The Eredivisie champions have handed the former Netherlands winger the responsibility of being in charge of the side's transfer dealings, youth academy and scouting duties
The 39-year-old recently left a similar position at Go Ahead Eagles, and the former Arsenal and Barcelona winger will now commence work at the Amsterdam ArenA.
In his new role, Overmars will mainly be focusing on the Eredivisie champions' transfer policy, youth academy and scouting matters.
The Emst-born Overmars wore the jerseys of Go Ahead Eagles and Ajax, as well as the Gunners and the Blaugrana during his playing career, while also making 86 international appearances for Netherlands.
He made 193 official appearances for Ajax, and won three Eredivisie titles, one Champions League, the Intercontinental Cup and one KNVB Beker with the Amsterdammers.