The classical singing duo will attempt to beat the current record held by Irish boyband Westlife, who visited five cities in 36 hours in 2002.
The pair will head to five cities in 24 hours on the release date of their second album 'Together Again', which is released on October 27, kicking off in Alfie's hometown of Blackpool before they hit HMV stores in Sheffield, Manchester and Nottingham to sign albums for fans.
Of the record attempt, Michael and Alfie said in a joint statement: ''We are ecstatic (and slightly nervous) to be taking on a new challenge, especially one that allows us to meet fans all over the country! What better way to celebrate the new album?''
Ball and Boe bring the West End, Broadway and Movie classics back to life on 'Together Again'.
The record features a wealth of hits from a 'West Side Story' medley to 'New York New York', As If We Never Said Goodbye and Bring Me Sunshine.
The second album is part of a partnership with Decca Records as the label announced three new signings: Michael Ball joins as a solo artist, Alfie Boe returns as a soloist, and Ball and Boe reunite as a duo.
The pair will also be returning to screens for their own ITV Special 'Ball and Boe Back Together' later this October, following the huge success of their first special last year.
The pair will bring their live show to arenas across the UK later this year, starting in Cardiff on November 30 and concluding at London's The O2 on December 14.
Information on how to gain access to the HMV signings can be found at www.hmv.com/hmvlive/michael-ball-alfie-boe
His new album Underneath It All is out now.