Law enforcement quickly arrested the man on suspicion of murdering his wife, decapitating her and attempting to burn the body, according to the Jerusalem Post.
Firefighters responding to an emergency call at the couple's apartment extinguished a fire and identified the headless corpse of a female victim in her 30s.
"A young ultra-Orthodox man was walking around the street with his wife's head in his hands, covered in blood. No one understood what was going on and why he had so much blood on him. Only later did they realize he was holding the woman's head," said a witness to the arrest, according to Israeli newspaper Maariv.
It was also reported that the alleged killer had claimed that he was the Messiah, and had visited a psychiatrist who subsequently released him, asserting that the man was not a threat to himself or others.
The crime comes on the heels of several high-profile cases of domestic violence in Israel.
A man in the town of Migdal, Israel, was indicted this month after admitting to murdering his wife, two sons, and a passerby in January.
On Sunday, prominent women's rights activist Siham Zabaraja was shot in her home, according to Jpost.com. Following her death on Tuesday, a gag order was issued concerning the details of the ongoing investigation.
According to Knesset Committee on the Status of Women and Gender Equality head Aida Touma-Suleiman, there is no "national plan" to address the murder of women in Israel.
"Women continue to pay the price with their blood and their lives," she said.