The Dutch were beaten on penalties by Argentina on Friday night in the quarter-finals of the World Cup, despite coming back from 2-0 down with seven minutes of normal time to go.
Van Gaal has admitted the loss was a tough one to take and, as planned, he is leaving his post with the Netherlands.
The 71-year-old, who was diagnosed with prostate cancer earlier this year, was appointed in August 2021 but agreed to only take charge until after the World Cup after previously being retired for five years.
“First and foremost I will not be continuing as a head coach for the Dutch team because I only did it for this period of time,” said Van Gaal.
“This was my very last match. My third term as a head coach. In that time I coached 20 matches but I didn’t lose a single one. I think it is Google you can look that up on. I am looking back on a fantastic period of time with a great group of players.
“I don’t think I’ve been beaten today, only in a penalty shoutout.
“I had a wonderful time and yes it is incredibly painful to see how we have been eliminated. Particularly as because I did everything to prevent this from happening.”