Well it's not clear whether it was radiation or FEV that mutated Harold. It's not far fetched to assume that the FEV vat chamber that Harold passed out in was also irradiated; in fact that's more likely since I don't see how the FEV could have affected him since he didn't fall into it like Richard Grey did. The FEV in Mariposa was a liquid; I doubt that the FEV evaporated thus becoming airborne since it was still there decades after the war.
It was the FEV... He only became the harold we know after a visit to Mariposa.
http://fallout.wikia.com/wiki/Harold
To the untrained eye, Harold appears to be an ordinary ghoul. This is not so, however. Ghouls are the result of massive radiation damage to a human body: Harold is a product of the Forced Evolutionary Virus. Unlike most people who are exposed to FEV, he did not become a super mutant, but is the result of a unique combination of radiation damage from constant low-level exposure, indirect exposure to FEV (It is unclear how Harold was infected with FEV as he blacked out for a while) and a fair amount of random chance. He's not a ghoul, and he's certainly not a super mutant. To quote Tim Cain, "Harold is special."
Furthermore, Tim Cain has this to say on the subject: "As for contact [with FEV], any contact at all will infect the subject, but the amount of contact determines the result. For example, I imagine Harold had some contact with the virus, but he was not fully immersed in it, so he became a different mutant than the Master's subjects. Full immersion, of course, is the preferred method of infection, as it provides the virus a large surface area for infection."
I'm just saying some developers once refered to him as a Ghoul, and he does use their sprite.