[5] Most of its art collection came from donations made by Alfred de Pass, a businessman and philanthropist who spent an important amount of his personal fortune on buying works of art, which were generously donated to museums and galleries throughout England and South Africa[6] The town's art collection, administered by the gallery's director Brian Stewart until his untimely death in 2010,[7] features works by major British artists including Sir Frank Brangwyn, Sir Edward Coley Burne-Jones, Charles Napier Hemy, Dame Laura Knight, Sir Alfred Munnings, Harry Ousey, William Strang, Henry Scott Tuke, John William Waterhouse, George Frederick Watts and Cornish painter John Opie.

[citation needed] Following a 2009 Art Fund bequest, Falmouth acquired a major collection including etchings by Pierre-Auguste Renoir and Edvard Munch, and several works by Prunella Clough, one of the most significant British painters and printmakers of the post-war period.

[citation needed] Falmouth also holds one of the most important master print collections outside London, including woodcuts, engravings, lithographs and screen prints by Albrecht Dürer, Rembrandt, Claude Lorrain, Adriaen van Ostade, Giovanni Battista Piranesi, Henri Matisse, Pablo Picasso, Francis Bacon, Merlyn Evans, Andy Warhol, Patrick Caulfield and Sir Peter Blake.

Groups such as Falcare, Age Concern, local schools and Falmouth University visit on a regular basis and create art in response to works on display.

In November 2021 to January 2022, the gallery hosted a collaborative group exhibition titled 'Thanks for the Apples', which featured nationally and internationally recognised contemporary artists including Nicholas Deshayes and Caragh Thuring.

The show was devised and produced by Naomi Frears and Ben Sanderson, who invited artists on a trip to Cornwall to visit the county's museums and explore their collections and archives.

From a hairball found inside a bull to a row of whimsy bottles and a tiny calendar, these artists focused their attention on objects and artworks that, while not hidden, can be overlooked, asking questions about the nature of these artefacts and what they might mean to people now.