The 29-year-old, who was released this summer by Fulham following their relegation to the Championship, will move to Villa Park on a two-year deal from 1 July.
The centre-back is due to fly to Brazil on Friday with the Swiss national side to take part in the World Cup finals, the third of his career.
Senderos, who spent six years at Arsenal between 2004 and 2010, spent the second half of last season on loan at Spanish side Valencia.
"I'm really delighted to be joining Aston Villa, a great club with such a big history, and for me this is a great step in my career," he told the official Aston Villa website.
"There will be a lot of competition for places with Ron Vlaar, Ciaran Clark, Nathan Baker and Jores Okore also very capable Premier League defenders, so it will be up to me to fight for and to earn my place in the team.
"This is a team and a club which wants to do better, I know this, and hopefully we can all develop together and create something special.
"My goal is to help the team keep as many clean sheets as we can and to help drive Villa where we deserve to be and want to be.
"I'm also excited to work with Paul Lambert whom I know has a great deal of respect also for Ottmar Hitzfeld (Swiss national boss who was Lambert's club manager at Borussia Dortmund) and my challenge will be to vindicate the trust he has shown in bringing me to Villa."
Lambert said: "He's played for some top sides and was a big influence in Arsenal's run to the Champions League final in 2006, so we're bringing in a really experienced player who's been there and done it and that will be important for the team.
"I went to Switzerland not long ago to watch the national team train and I could see he has a good, strong mentality for the game. Ottmar knows players and for him to say that Philippe has never disappointed him on the pitch, that's no small commendation.
"This will be Philippe's third World Cup finals and there aren't too many players who compete at that level over that stretch of time. He'll be a great addition to the group."
Senderos began his career with Servette before moving to Arsenal in 2004. Loan spells at Milan and Everton followed before he joined Fulham on a permanent deal in 2010.