Bond, 58, joins the Italian, who was announced as boss at Villa Park on 2 June, with former Reading manager Steve Clarke, 52, named as his assistant.
Villa were relegated from the Premier League in April, finishing on just 17 points.
Chinese businessman Dr Tony Xia agreed to buy Villa for £60m in May.
Bond was reserve team coach under Harry Redknapp at Portsmouth, before following him to Southampton to work as coach in 2004. The pair returned to Fratton Park a year later, and Bond joined Redknapp at Tottenham in 2008 and QPR in 2012.
Clarke, who was sacked as Reading boss in December 2015, previously managed West Midlands rivals West Brom.
Italian Massimo Battara is the club's new goalkeeping coach, while compatriot Massimiliano Marchesi has been appointed fitness coach.
Battara has experience at Napoli, Fiorentina, Inter Milan and Manchester City, and worked with Di Matteo at Bundesliga side Schalke.
Marchesi's most recent job was at Italian giants Inter having worked in the Middle East for 10 years.
Aston Villa have appointed former Tottenham and QPR first-team coach Kevin Bond to work alongside new manager Roberto di Matteo.