Freeman, best known for his work in The Office, Sherlock and The Hobbit, will be joined in the cast by Gina McKee as Queen Elizabeth.
McKee was last on stage last year in Di and Viv and Rose at Hampstead Theatre. Her other credits include Michael Grandage's productions of King Lear and Ivanov for the Donmar. On screen she is best known for Notting Hill and more recently TV series The Borgias.
Additional casting includes Simon Coombs (Tyrrel), Philip Cumbus (Richmond), Gerald Kyd (Catesby), Paul Leonard (Stanley), Forbes Masson (Hastings), Paul McEwan (King Edward IV/Bishop of Ely), Mark Meadows (Clarence/Lord Mayor), Lauren O'Neil (Lady Anne), Maggie Steed (Queen Margaret) and Jo Stone-Fewings (Buckingham).
Design is by Soutra Gilmour, who collaborated with Lloyd on the first Trafalgar Transformed season.
Tickets for Richard III, which runs from 1 July to 27 September 2014, will go on sale on Tuesday 13 May at 10am.
The second Trafalgar Transformed season, like the first, will offer £15 Monday tickets for all productions, applicable on all seating within the theatre, further encouraging first-time theatregoers to experience the exciting programming at the venue.
The production will be accompanied by a programme of 'Traf Extras', including debates, post-show Q&As and rehearsed readings.
Further productions in the second Trafalgar Transformed season are expected to be announced imminently.
Lloyd's previous season of Trafalgar Transformed - so named following refurbishment of the space to include a raised stage and new seating - included Macbeth starring James McAvoy, The Hothouse with Simon Russell Beale and The Pride featuring Hayley Atwell.
His other recent productions include the UK premiere of Urinetown, which recently completed its run at St James Theatre and has been tipped to transfer to the West End later in the year.