The 39-year-old had spent just three days with her four-year-old Gabriella and was given hope there would be an extension to her release from prison.
However, despite promises from prosecutors that her furlough from jail would be extended, hours later she was back behind bars.
Her husband Richard Ratcliffe revealed the heartbreaking news that his wife had been taken back to prison.
He said: "Nazanin waited for Gabriella to wake up before saying goodbye, and left her family home to return to Evin prison.
"She promised Gabriella that the next time she saw her it would be forever not just for a few days, for proper freedom, not just for furlough. And next time they will go back to London to be with daddy."
Nazanin decided to go into the prison voluntarily rather than be dragged out of the house in front of Gabriella when the Iranian authorities refused to prolong her release.
The mum, from Hampstead, north London, was sentenced to five years in jail after being accused of spying by Tehran's Islamist regime.
Earlier she was clearly overjoyed to be out of custody, Richard revealed in an interview with Radio 4 this morning.
He said: "She was euphoric on the first day and the second day at just being out of prison and seeing the family.
"I spoke to her on Skype (it was) the first time I had seen her in more than two years. She had a big grin on her face."
However, when she headed back to prison her husband said it felt like the family had hit a "brick wall."
Jeremy Hunt has given the case of Nazanin Zaghari-Ratcliffe greater priority than his predecessor as Foreign Secretary, the imprisoned charity worker's husband has said.
Richard praised Mr Hunt for being "clear and critical" about his wife's case, after she voluntarily returned to prison in Iran following an emotional family reunion over the weekend.
Mr Ratcliffe suggested there had been a change in the relationship with Iran since Mr Hunt replaced Boris Johnson as Foreign Secretary last month.
And he said he had "sensed a change in the way he has prioritised Nazanin's case".
"I think one of my complaints with the Government was that it didn't feel like it was sort of treating her case with the public severity that I thought it deserved," he said.
"He's been great in that sense: he's been clear and critical and he's said 'listen, she's innocent and she shouldn't be in prison, her treatment has been appalling', and all the things that we've been asking the Government to do."
Mr Ratcliffe added: "In terms of how the relationship with Iran has changed, well clearly she got out for a few days, that's a pretty good sign and there have been some other improvements."
On Sunday, Mr Hunt said he had spoken to Iran's foreign minister Mohammad Javad Zarif on Friday but that it "clearly wasn't enough".
Vowing to continue the fight, he tweeted: "Looks like Iranian legal system is impervious to the simple fact at the heart of this: an innocent woman is desperate to be reunited with her family."
Richard, who has been unable to get an Iranian visa, said his wife's temporary release initially appeared to be a "very good sign", but said it felt "pretty cruel at the end of it".
He added: "It was a slight surprise that she was released but it felt consistent with positive noises, so it wasn't just a bump, it was a proper brick wall yesterday that she was brought back in."
Touching images taken earlier this week showed her cradling Gabriella in her arms in Damavand at the start of her release from prison.
She was also seen kissing her daughter, who famously asked former Foreign Secretary Boris Johnson to help free her mum.
While out, Nazanin and her daughter were able to go on an outing to a coffee shop to talk with her husband Richard over Skype.
Before embracing her daughter, Nazanin said: "The thought of brushing her hair, giving her a bath, of being able to take her to the park, feed her and sleep next to her – it just kills me.
"It is still so hard to believe."
Kate Allen, UK Director of human rights group Amnesty International said Nazanin's return to prison was a "crushing disappointment."
She said: "We shouldn’t lose sight of what Nazanin has had to endure – nearly two-and-a-half years behind bars, eight gruelling months of solitary confinement without a lawyer, a deeply unfair trial, and also being subjected to a string of unfounded accusations from the Iranian authorities."
The human rights campaigner added that Nazanin was a "prisoner of conscience who should never have been jailed" and called on the Government to do everything it can to secure her release.
Former BBC employee Nazanin was sentenced to five years behind bars in 2016 after being accused of plotting to overthrow the Iranian government.
She was arrested at Tehran airport after flying in for a holiday with her daughter and locked up in solitary confinement for 45 days on spying claims.
Nazanin was summoned by prison officials while still in her pyjamas and told she had just 10 minutes to get ready for her brief release.
With her cellmates gathered round the cramped cell, she dressed and packed in a flash before guards painstakingly searched every item she was taking out of prison.
Once dressed, Nazanin, who was forbidden from calling her family from Evin prison, was taken to the front gate where some of her relatives had already gathered.
Her brother then took her to the city of Damavand where some of her wider family was celebrating Eid – and where her beloved Gabriella was waiting eagerly with flowers she had picked from the family garden.
An overwhelmed Nazanin burst into tears at the sight of her family, according to the Free Nazanin campaign spearheaded by her husband Richard.
She later said: "I wasn’t expecting it at all when it was mentioned two weeks ago.
"I didn't tell Gabriella or for a long time or my mum – so if it didn’t happen I would be the only one to suffer.
"I was so emotional to see my grandmother today. I cried so much. I felt so overwhelmed.
"My dad’s home is not my home – but it is so much better than prison. People in the ward were so excited – they sang songs and danced.
"I baked for them in celebration. It felt like this really could be the beginning of the end."
And her husband Richard added: "Despite the build up, today was a genuine surprise after all the disappointments.
"We have been burned by hope before, so it had been easier to presume disappointment would come again.
"But it didn’t – she is outside those prison walls. And we are all so pleased."
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