The 39-year-old TV presenter was overcome with emotion after speaking to Sister Gabriel and Sister Geraldine-Marie of Poor Clares of Arundel, whose album Light For The World recently topped the UK classical music charts.
Willoughby had to ask co-host Phillip Schofield to read her lines from the autocue for her after bursting into tears.
'If you're at home and you're fed up ... or feeling depressed ... we're here, and we're with you'
Sister Gabriel and Sister Geraldine-Marie made @hollywills tear up today with this emotional message.
Watch their full interview on the ITV Hub 👉 https://t.co/1VuxanpnIc pic.twitter.com/sBfS9RftST
— This Morning (@thismorning) January 26, 2021
She said: "Some people just talk and they really get you, don't they? Oooh, that took me by surprise.
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Fanning her face she sobbed: "It's when somebody says it's all going to be okay…"
Willoughby told Schofield: "You're going to have to do this bit."
When the cameras returned to Willoughby, she reassured viewers: "I've pulled myself together now."
Sister Gabriel and Sister Geraldine-Marie, from the south east of England, were on the ITV daytime show to discuss their choir, which has proved popular for those seeking reassurance and hope during the coronavirus pandemic.
They said: “We are really thrilled that something of the essence of our life is helping people.
"We just want to say hat when you listen to our CD if you're at home and you're fed up, or anxious, or feel depressed - somewhere in Arundel in West Sussex there's a community of women.
"We're here, and we're with you. We're making this journey as well."
Willoughby - who has three children, Harry, 11, Belle, nine, and Chester, six with production company boss Dan Baldwin - has admitted to struggling with juggling work and homeschooling during the country’s third national lockdown.
She recently shared a picture of herself reading to youngest son Chester on Instagram, captioned: “Eat, Sleep, Read, Repeat...”
Watch: Holly Willoughby speaks about mental health during lockdown