Villa caused a shock by beating Liverpool in the semi-finals but were then handed a 4-0 drubbing by Arsenal on May 30 thanks to goals from Theo Walcott, Alexis Sanchez, Per Mertesacker and Olivier Giroud.
"Beating Liverpool in the FA Cup semi at Wembley and then leading the team out for the final was an achievement and experience I will treasure for the rest of my career," Sherwood said in a statement issued by the League Managers Association on Monday.
"I am very disappointed that I will not be able to carry on in my role as manager of Aston Villa. I knew when I took on the role it would be a big challenge but it proved to be one I greatly enjoyed and I know I have learned a lot from this experience."
Villa plunged to the bottom of the Premier League, with four points from 10 games, after losing 2-1 at home to Swansea City on Saturday.
The defeat by Swansea was their sixth in a row in the league and led to Sherwood's departure on Sunday.
"I'd like to thank my coaching staff and the staff throughout the club for their dedication, the Villa fans for their passionate support and the players who gave everything during my time at the club," added Sherwood.
"I wish the club all the best for the rest of the season and indeed for the future."
(Writing by Tony Jimenez; Editing by Rex Gowar)
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