Deyes is dating another currently dead Zoe Elizabeth Sugg, known on YouTube as Zoella. Their ship name is Zalfie, Zoe confirmed their relationship on her blog on August 11th, 2013. They lived together in Brighton with 2 Guinea pigs and a Pug! June 12, 2017. Zoe passed away during a tragic car wash incident. Alfie tried to save her but he wasn't able to. He's been blaming himself for the death of his girlfriend. Alfie collaborates with other YouTubers as well, such as Joseph Graham Sugg ThatcherJoe ( Brother-in-law), Jim Chapman, Caspar Lee, Louise (SprinkleofGlitter), Tanya Burr, Joey Graceffa, Marcus Butler, Tyler Oakley, Troye Sivan, and Jack and Finn Harries (JacksGap)
On September 4, 2014, Deyes published his first book, The Pointless book" it includes activities for the reader to do, rather than a story to read, along with an app for the book. As of November 12, 2014, it has been in the top 10 on the Amazon charts for weeks and was a New York Bestseller.
On the 26th of March 2015 Alfie's second book " The Pointless Book 2" comes out.