A statement released by Lebanon's Internal Security Forces, ISF, said the Syrians were arrested in the Asian nation's eastern region, after entering the nation irregularly.
The pair were part of a network that smuggled "hundreds" of people including "Syrians, Lebanese, Egyptians, Palestinians" and others of unspecified African nationalities from Libya to Europe by boat, the statement added.
They admitted to asking $3,500 per person and to organizing boat trips towards Italy and Greece.
A boat they had arranged "sank off the coast of the Libyan city of Tobruk" in the country's east, resulting in "dozens of deaths," according to the statement, and the duo subsequently fled Libya for Syria.
One of the arrested suspects worked with his brothers in Libya and Greece, the statement said, adding that the men had accomplices "in Lebanon's Wadi Khaled area," a key location for irregular crossings from Syria.
Libya is a major gateway for migrants and asylum seekers attempting perilous sea voyages in often rickety boats in the hope of a better life in Europe. The central Mediterranean route has been dubbed the world's deadliest sea crossing for migrants.
Lebanese authorities ramped up efforts to confront irregular migration, and report preventing thousands of illegal crossings through Lebanon's porous border with Syria in recent weeks.
Lebanon's economy collapsed in late 2019, turning the country into a launchpad for migrants.
Lebanese nationals have increasingly been making the treacherous voyage towards Europe alongside Syrians fleeing war and economic woes in their country, as well as Palestinian refugees.
Migrants seeking to reach Europe from Lebanon generally head for the east Mediterranean island of Cyprus less than 200 kilometers (124 miles) away.
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