Staff at the British Heart Foundation shop in Penzance have said they were "blown away" by the recent donation from islanders.
Jo Legg organised a donation drive for the charity in February following a successful collection for Cornwall Air Ambulance last year.
The Penzance store has now thanked Jo, the islands' community and the Isles of Scilly Steamship Group, which provided free transport, "from the bottom of our hearts".
They wrote on social media: "There [has] been a flurry of activity in our shop in the last few days!!!! Lovely Jo Legg from the Isles of Scilly has very kindly organised a stock generation event for BHF on the island.
"We have been friends with the lovely islanders for many years and were always humbled by their generosity and community spirit but we were absolutely blown away by this donation.
"Jo and the residents of St Mary's filled 2 and a half containers, floor to ceiling, with clothes, shoes, books, DVDs, bedding, toys, homeware and every other thing imaginable!!! Utterly amazing !!!! We are in awe of the amount of work and passion that went into completing this project!
"Massive thank you to Jo, amazing community of Scillies and to Isles of Scilly Steamship Company very generously providing the transport and storage free of charge. Thank you from the bottom of our hearts xxx."
Goods donated by Scilly residents raised more than £10,000 for Cornwall Air Ambulance in February 2018.