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The defections came as Juan Guaido, the country’s opposition leader, called on security forces to abandon Mr Maduro and to allow humanitarian aid into the nation – amid violent clashes at the border that saw two people killed and one shipment burned.
Mr Guaido declared himself interim president a month ago but has so far been unable to win support from Venezuela’s military, which remains loyal to the Maduro government.
Some 104 soldiers have now fled across the border into Colombia, according to CNN en Español and the Agence France-Presse news agency.
On Saturday at least two people were killed near the Brazilian border while 300 were wounded in a separate clash at the country’s border with Colombia after civilians fought with troops loyal to the president.
On Sunday Brazil responded to the rapidly escalating violence by calling on the international community to join in the “liberation effort” of Venezuelans.
Meanwhile, Mike Pompeo, the US secretary of state, said that Mr Maduro’s ”days were numbered”.
His comments come as Mike Pence, the US vice president, prepares to meet regional leaders in Colombia on Monday to discuss the violence.
Mr Pence will announce "concrete steps" intended to address the crisis according to a senior US administration official.
Nicolas Maduro has refused US aid shipments and claims that the supplies are part of a coup attempt against him.
He has closed the country’s borders with Colombia, Brazil and the island of Curacao, effectively severing any path for food and medicine supplies to enter the country.
On Saturday Mr Maduro also broke off diplomatic relations with Colombia and accused the country of assisting a US-led effort to remove him.
For weeks the US and its regional allies have been amassing aid at Venezuela’s borders with the aim of launching a “humanitarian avalanche”.
On Saturday Mr Guaido made numerous appeals to troops at border bridges, as he tried in vain to persuade them to allow aid into the country.
“How many of you national guardsmen have a sick mother? How many have kids in school without food?” he said, standing near a warehouse in the Colombian city of Cucuta, where 600 tons of food and medicine have been stockpiled.
“You don’t owe any obedience to a sadist ... who celebrates the denial of humanitarian aid the country needs.”
The opposition politician also urged the international community to keep ”all options open” in the fight against Mr Maduro, following Saturday’s violence.
Mr Guaido encouraged civilians to gather at border bridges on Saturday but the crowds were driven back after troops fired tear gas at protesters, triggering a stampede at least one location.
Analysts say that there may be no clear victor in the clashes and humanitarian groups have criticised the opposition for using the aid as a political weapon.
International leaders including UN secretary-general Antonio Guterres are appealing for the sides to avoid violence as the political standoff continues.
Additional reporting by agencies