With this, the 47-year-old Santo will lead the Wolves for the last time against Manchester United on Sunday in the final round of the Premier League.
The end of a four-year journey in which Santo, a former coach of Porto, Valencia and Rio Ave, made 198 matches for Wolverhampton, winning 96 of them and losing 56.
Santo worked as a goalkeeper coach in a technical apparatus led by former Zamalek coach Jozwaldo Ferreira, in Malaga and Panathinaikos.
Reports said Santo, the former goalkeeper for Deportivo La Coruna and Porto, is a candidate to lead Tottenham, who earlier dismissed coach Jose Mourinho.
Ryan Mason leads Tottenham on a temporary basis until the end of this season.