Suspect Nalah Jackson was arrested at approximately 2pm on Thursday by officers with the Indianapolis Metro Police Department (IMPD) after officials received several tips that she was in the area, said Columbus Police Chief Elaine Bryant during a news conference.
The mother of the children, Kason and Kyair Thomass, was picking up a restaurant order while working as a DoorDash driver and left a black 2010 Honda Accord running outside a pizzeria on High Street in Columbus on Monday night, CNN previously reported.
When she came out, the car was gone. Kyair was later found abandoned near the Dayton International Airport at around 4.15am on Tuesday.
"At this moment, she is being questioned by police. However, Kason Thomass was not with her at the time of her arrest," Bryant said, adding that officers have been working "around the clock" since the twins went missing on Monday.
"We will not stop until we find Kason," the chief said. The FBI is offering a $10,000 (A$15,000) award for the safe return of Kason, she added.
Since Jackson crossed state lines, she will be facing federal charges, Bryant said.
"It will absolutely be a federal investigation," she said.
A warrant for Jackson's arrest was filed through the Franklin County Court, according to an online docket. An Amber Alert went out for the twins at 1.37am on Tuesday, officials said.
Restaurant employees told police that a homeless woman exited the restaurant after the twins' mother entered the restaurant.
The individual was later caught on camera at a gas station where she asked an employee for money.
Witnesses spotted suspect
Columbus Police Deputy Chief Smith Weir said during the Thursday news conference that officers have received "over three dozen tips" since Wednesday from throughout the state.
Late on Thursday morning, the department's hotline received several calls from people in Indiana who believed they spotted Jackson in Indianapolis and officers "implored" the witnesses to call 911. IMPD informed Columbus police around 2pm that they had stopped an individual who they believed to be Jackson and both departments worked together to identify her before taking her into custody, Weir said.
"If you have any information regarding this crime or the whereabouts of this baby, please contact us as soon as possible," Weir said, adding that three detectives from the Columbus Division of Police are traveling to Indianapolis to coordinate with IMPD and the FBI to further the investigation.
Indiana will issue an Amber Alert asking for information that could help locate Kason and the missing vehicle, Weir said.
Family pleads for the child's safe return
Earlier Wednesday, family members and community leaders gathered to pray for the safe return of the child.
During the vigil, the twins' grandmother, LaFonda Thomass, begged for the return of Kason.
"If you look at him and you see anything, see a precious child who's longing for his mother," she said. "We beg you, please, please, please do the right thing and just bring my baby home."
First Assistant Chief of Police LaShanna Potts said during the vigil, "We are committed to finding baby Kason. We want Nalah to do the right thing. … We know she's capable of doing it because she did release one baby."
Officials are asking people to be on the lookout for a black Accord with a torn Ohio registration sticker on the rear bumper and a white bumper sticker that says, "Westside City Toys."
The vehicle was recently purchased and did not have a license plate, which made it harder to track, Weir said.
"I plead to you, please return Kason Thomass. We thank you for returning Kyair. You've already shown us you can do the right thing. You can return him to any safe location," Bryant said during a news conference Tuesday.
Officials do not believe there's a connection between the twins' family and the suspect.