The suspension came a day after Germany's Lufthansa said it would suspend its services to the country.
The German company said Venezuela owed it millions in ticket revenues.
Oil-rich Venezuela has been hit hard by the global drop in oil prices and suffers from high inflation and a chronic shortage of basic goods.
Several airline companies have said that currency controls in Venezuela made it impossible for airlines to convert their earnings into dollars and send the money abroad.
In a statement, Latam airlines said it would suspend its operations to Caracas airport "temporarily and for an unspecified time".
It said flights on its Sao Paulo to Caracas route would end first, within days, and the other routes it runs to Caracas from Lima and Santiago would be halted by the end of July.
Strict currency controls were first imposed in Venezuela in 2003 by late President Hugo Chavez.
The restrictions were further tightened two years ago, forcing several airlines to reduce their operations in the country as they struggled to repatriate billions of dollars in revenue held in the local currency - the bolivar.
Some airlines are now requiring passengers to pay their fares in dollars.
Venezuela's government says it is using its foreign reserves - which are now scarce - to pay for essential items such as medicines and industrial machinery.
Recently Coca-Cola said it would be halting production of some of its soft drinks because of a lack of sugar while the tyre and rubber products company Bridgestone also ended its more than 60-year relationship with the country.

Innogy Renewables UK Ltd had been proposing a hydroelectric scheme on the River Conwy, near Betws y Coed in Snowdonia National Park.
But on Wednesday it said it had decided to shelve the Conwy Falls project.
The application had been due to be considered by Conwy council planning committee next week.
Innogy Renewables UK said the decision to withdraw the application was made following a late request for additional information.
It said that Natural Resources Wales' river basin management plan for western Wales had been updated last December, including a change to the sensitivity of salmon fisheries, following which further information had been requested.
The project, providing power to 3,200 households, attracted opposition from environmentalists, anglers, canoeists and businesses.
The firm has previously said it would have had a positive impact on the environment but campaigners were worried half an acre of the centuries-old Fairy Glen Wood would be destroyed by the build.
In March, the park's authority turned the plans down, asking for clarification on "minor issues".
Innogy Renewables UK Ltd said it would now consider its next steps.
Conservation charity the Snowdonia Society said it was "relieved that the immediate threat to the wonderful Conwy Falls and Fairy Glen has passed, but concerned that it could resurface yet again".

The result means the Senegalese join Zambia as the only African sides in the round of 16.
South Africa and Guinea are already on their way home after being eliminated from the tournament.
Senegal put the ball in the back of the net after 54 minutes but the video assistant referee ruled that Aliou Badji's effort was illegal as the forward had fouled Ecuador goalkeeper Jose Cevallos.
Senegal finished the match with 10 men after Cavin Diagne was sent off following a second bookable offence.
The share of the points in Jeonju means that Senegal finish as Group F runners-up to the United States who drew 1-1 with Saudi Arabia in the group's other match.
Next up for Senegal is Mexico while Zambia will face Germany.
The largest airline in Latin America, Latam, says it is suspending its flights to Venezuela because of the worsening economic situation.
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Controversial plans for a £12m renewable energy project at a Conwy county waterfall beauty spot have been withdrawn.
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Senegal are through to the second round of the Under-20 World Cup in South Korea after a goalless draw with Ecuador.