The 'Kiss You' singer - who split from the 23-year-old country music star in January after two months together - reportedly refers to their romance as a "pain in the a**e" and claims he hasn't dated anyone he wanted to have a serious relationship with since becoming famous.
According to the Daily Star Sunday newspaper, the 19-year-old British heartthrob admits in the band's documentary: "I haven't met a girl yet who I'd want to even think of getting serious with.
'"I think I've been unlucky in love so far. But then, I haven't really met anyone who's made the earth move for me.
"I'm longing to meet someone who really inspires me and makes me really want to spend time with them."
The 3D movie, which follows Harry and his band mates Niall Horan, 19, Zayn Malik, 20, Liam Payne, 19, Louis Tomlinson, 21, as they tour the world, is set to be released in August.
Harry split from Taylor, who penned her hit 'I Knew You Were Trouble' about him, after they had a massive bust-up on the British Virgin Island, Virgin Gorda in early January and she fled their plush resort early.
She has since been linked to Hawaiian surfer John John Florence, while Harry recently struck up a flirty friendship with Kesha via text message.