The company said it is aiming to provide the network to approximately 70% of the population by 2018, however there are concerns that users will be put off by a high price tag.
The service will cost subscribers approximately $50 a month, in a country where the average minimum wage equates to $215.
It will be offered under the Tigo brand, and is presently available to over 50% of the country’s 10.5 million population.
The company is aiming to extend coverage to 170 municipalities, addressing 70% of the population by 2018.
"Today's launch of the super high-speed service in Bolivia is our latest innovation in the country following the launch of our satellite TV service there in April," said Millicom CEO Hans-Holger Albrecht. "It represents our commitment to transforming lives with the digital lifestyle and we hope that people in Bolivia will enjoy its benefits over the next few years."
Millicom launched its first 4G network in Colombia in December last year.