The woman was filmed walking around and shouting outside the Oktyabrskoye Pole metro station.
Russia's Interior Ministry released a statement saying they believed the head belonged to a four-year-old girl who the woman had been babysitting.
The girl has been identified as Nastya M.
Her babysitter has been named as Gyulcherhra Bobkulova, from Uzbekistan.
Earlier on Monday, police found a headless child's body in an apartment after a fire, Russian news website RBC reported.
The woman is said to have appeared near Oktyabrskoye Pole metro station in northwest Moscow.
Moscow investigators said in a statement the unnamed nanny was from Central Asia and that she was undergoing psychiatric testing to see if she was mentally sound and understood the significance of the crime they said she had committed.
The woman was reportedly seen pulling the chopped-off head out of a bag.
Then she began shouting about killing the child and that she would blow herself up.
She was seen praying shortly before police arrested her.
The nanny has been identified as Gyulchehra Bobokulova, from Uzbekistan.
Dramatic CCTV footage has captured the moment police swooped and dragged the woman to the ground in a tense stand-off.
Eyewitnesses at Oktyabrskoye Pole underground station said the woman yelled: "My child was killed… I will blow up everyone…"
She also shouted: "I hate democracy."
Witness Alyona Kuratova told Russia's Rain TV: "I came out of the shopping center and they tried to not let me through. There were a bunch of people there, running, screaming 'bomb, bomb'.
"I saw that a woman was walking near the Oktyabrskoye Polye metro, near the road, all in black. She had not even some kind of bundle, but a head.
"Maybe it was a child's head, like they were whispering in the crowd. She was shouting something."
A preliminary investigation revealed that the suspect is a children’s nanny in her late 30s, who is a citizen of a “Central Asian country".
Investigators claim that the baby sitter waited until the parents of an older child had left the apartment before murdering the child and starting a fire.
The source in the Investigative Committee of Russia said: "She waited until the parents with the elder child left the flat, then for unknown reason she killed the child, set fire to the apartment and left the scene.
"She was detained at the metro station Oktyabrskoe Pole."
Женщину у метро «Октябрьское поле» задержали по подозрению в терроризме https://t.co/6tI1RNRCEgpic.twitter.com/0UAEQp8Ao1— #говоритмосква (@govoritmsk) February 29, 2016
The dead child is understood to have a 15-year-old brother and her family from the Oryol region was renting the apartment.
Her mother reportedly works at a wedding shop while her father is understood to be a technician at a mobile phone company.
The child's mother was taken to hospital in an unconscious condition after she learned of the news, according to reports.
The woman was reportedly drugged, a police source said.
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