The 49ers cruised to a 42-10 win over the winless Jacksonville Jaguars in the second game of the International Series.
Harbaugh told reporters: "It was a great environment. It felt like a huge stage. Wembley has a great tradition and status as a venue and it was an amazing experience for our players and me personally.
"The beginning of the game when they were playing the two national anthems, I felt like I was at the Olmypics.
"As a youngster, I always wanted to be in the Olympics and at that moment I was feeling like the moment when they play the gold medal, the silver and the bronze medal, the different anthems.
"I got a chill when the gal was singing "God Save The Queen".
The 49ers are 6-2 in their season after week eight.