Both stars were appearing on Channel 4's Sunday Brunch – with 29-year-old Bebe appealing for a British boyfriend.
Taking part in the cooking segment of the show, the blonde beauty joked: "Are there any cute, single, English guys out there?"
Poking fun at her inability to carry out the task at hand, she added: "That wants a girl that can cook?"
From across the studio, Olly raised his hand and exclaimed: "I'm over here!"
However, the singer's advances were awkwardly rejected by Bebe, who quickly rebutted his offer and said: "I won't date another singer."
Olly was left red-faced after being jilted, with hosts Tim Lovejoy and Simon Rimmer gasping at Bebe's comments.
They retorted: "Olly Murs is a national treasure – you'd be lucky to have him!"
To which the Essex-born star replied: "You will not be lucky to have me, let me tell ya."
He then joked that any women who are interested in dating him should "get on Tinder", with Bebe asking single, male viewers to tweet in a selfie to the show so that she could have her pick of the bunch.
Viewers at home were stunned by Bebe's snub and took to social media to share their thoughts.
One fan wrote: "Olly Murs just got owned on #SundayBrunch!"
Another tweeted: "I would definitely go on a date with Olly!"
Olly has been single since 2015, when he broke up with his long-term girlfriend Francesca – which he has previously confessed that he regrets.
Speaking about the end of the romance, he said that at the time he was putting himself and his career first, which meant he didn't prioritise his relationship.
He told Fabulous: "I was a young pop star, and what came with that was a lifestyle of me putting myself first.
"I don't feel like I treated my ex-girlfriend badly – I treated her well, actually. It was a good relationship, but my priorities were different to what they would be if I was with someone now.
"I think if I could go back, I would have put her first more. When I got with her, Troublemaker [Olly's 2012 platinum-selling No.1 single] had just come out, which was like a f**king sky rocket, and it was selfish of me, but that was the way it was.
"I was on this f**king rocket and you only get one chance at this so you have to go there."
Olly previously joked that he might fall in love with a contestant during his stint as a judge on The Voice UK.
He quipped at the time: "Spinning these chairs could be the only way I ever could find love."
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