The result means the Black Cats are without a win at home since December 17 last year and have just one victory from 15 Championship games this season, leaving them inside the relegation zone.
Grayson was appointed in June and was expected to stabilise a club that had been relegated from the Premier League with just 24 points.
In a statement posted on the club website in the immediate aftermath of the game against bottom-club Bolton, chief executive Martin Bain said: "Simon and his team have worked tirelessly to achieve the best for the football club during their time here.
"While we hoped that Simon’s experience in the Football League would help us to a successful season, results have not been good enough for a club of this stature.
"In order for us to improve upon our current position we believe a fundamental change is necessary."