In 2008, during an interview for The Skeptics’ Guide to the Universe, he describes Captain Disillusion as a YouTube web series that tackles paranormal and illusion videos uploaded by others on YouTube. He started this effort as a blog entry on Myspace but later saw these items as ready made scripts for short videos. He notes that Penn & Teller were instrumental to his current interest and eventually found the skeptical movement involved in similar work. He finds that his followers like to learn about the illusions. It is not his intent to spoil legitimate entertainment or spoil a current performers work. His intent in showing how video illusions are created is to clear up misconceptions. Melikdjanian describes the basis for Openfilm.com briefly, saying it “was formed for film makers. The goal is to provide higher quality product and a group of serious content creators.”

During an interview for The Skeptic Zone, in 2010, he describes Captain Disillusion as a superhero. and in a following 2011 interview, he describes his work as Captain Disillusion is done “in the maximum fun way possible”. He describes his work with James Randi, Randi calling him to participate in The Amaz!ng Meeting and his video work with Randi in a later project. During an interview by Susan Gerbic for Skeptical Inquirer, he states “I think it’s best to focus on what you know—something you’re already an expert on outside of skepticism—and explore the ways in which it’s connected to skepticism. With Captain Disillusion I connected a random thing—visual effects—to skepticism in a way that people seem to find engaging. I’m sure that can be done with many other fields in different ways.”

In 2011, Melikdjanian released a DVD of his Captain Disillusion series, entitled Captain Disillusion – Fame Curve Collection. It contains the first 16 episodes remastered with optional commentary and additional bonus features. He debuted it at TAM9, and later made it available for purchase online.

Melikdjanian was the co-founder and creative director of FilmNet.com, and was the co-founder and chief creative officer of Openfilm. Both were intended as alternatives to popular video-sharing site YouTube, but for serious amateur filmmakers who “don’t want to place their work alongside YouTube’s mediocrities.” OpenFilm closed in August 2015.

In a 2017 interview with Richard Saunders from The Skeptic Zone, he said, when talking about the video effects editing process that “You know, the tools change but the methods really don’t. It’s all about making things look questionable and kinda crappy and low quality and then you can pretty much get away with anything”. In replying to a follow up question regarding believing what you see on the internet he said “When I started out, people just kinda believed everything, it was like shooting fish in a barrel, but these days people are just really asking me “is this fake?”, “is this fake?”, “is this fake?” and half the stuff they show me is just you know, a juggler juggling a lot of balls. They can’t conceive that that could be real, people just don’t believe anything anymore. I guess that’s good for me because I get to explain lots of stuff but I wish people could finally strike that balance where they’re not too credulous but they also know not to just dismiss everything out of hand”.