Two senior security officials said al-Assir was detained on Saturday at Beirut's Rafik Hariri International Airport as he was trying to flee the country in a disguise and using a forged passport.
Security sources added that Assir, who had shaved his beard, was trying to fly to Egypt.
Assir has been supporting foreign-backed terrorists in Syria since the war began in the Arab country in 2011.
In June 2013, 12 Lebanese soldiers were killed when Assir and a number of others opened fire on the soldiers in the southern city of Sidon.
In 2014, a military judge recommended prosecutors seek death sentences for Assir and 53 others, including former singer Fadel Shaker.
He and his associates were accused of "having formed armed groups that attacked an institution of the state, the army, killed officers and soldiers, took explosive materials and light and heavy weapons and used them against the army".
He had been on the run since then.