"I would go further than the President" in the two-year conflict between Syrian rebels and forces loyal to president Bashar Assad, Levin said during a speech at the Council on Foreign Relations on Monday.
The Michigan Democrat also proposed the United States and its allies begin "going after" Assad's anti-aircraft defenses and the government's formidable air power arsenal, which has decimated rebel forces and civilians alike during the conflict.
Attacking Assad's air defenses and creating a safe zone near Turkey have been championed by Levin's Republican colleagues on the Senate defense panel in recent months, with GOP Sens. John McCain (Ariz.), Lindsey Graham (S.C.) and Kelly Ayotte (N.H.).
Such efforts, according to Levin, would help contribute to a "good aftermath" in Syria were a burgeoning democracy can flourish once Assad falls.
The worst case scenario, he noted, would be if the ensuing power vacuum in a post-Assad Syria sparks secretarian infighting among rebel factions and opens the door for groups like al Qaeda to take hold in the country.
However, the options outlined by Levin on Monday would likely require the White House deploy U.S. warplanes into the region, escalating American military involvement in a conflict that the White House is seeking to resolve by diplomatic means.
While Levin did express his support for the no-fly zone in Turkey and to take out Assad's air assets, he admitted such actions would not guarantee an end to the violence in Syria.
"I am not certain, believe me, to say I have a 100 [percent] confidence as to what the right road is" in Syria, Levin said regarding his remarks during Monday's speech.
But the longtime Senate defense committee chief did side with the Obama administration's decision not to directly provide weapons to Syrian rebel factions.
The Obama administration has balked at arming Syria's rebels, over fears those weapons would end up in the hands of Islamic militant groups that have worked their way into the opposition's ranks.
Gulf states, such as Oman and the United Arab Emirates, have supplied arms to rebel forces with France and the United Kingdom possibly following suit. Former Defense Secretary Leon Panetta backed arming Syria's rebel forces during the waning days of his tenure at the Pentagon.
Rep. Eliot Engel (D-N.Y.), ,the top Democrat on the House Foreign Affairs panel, will introduce a bill on Monday demanding the White House to provide up to $150 million in lethal and non-lethal security assistance to “appropriately vetted” groups seeking to overthrow Bashar Assad's regime.
For his part, Levin said "the president's approach to Syria has been the right approach," on the decision to deny American arms supplies to Syrian rebel forces, opting rather to provide diplomatic support to "those forces we believe will be the right forces . . . that will bring together all elements in Syria."
"To accomplish that goal [Obama] has to be careful into whose hands advanced weaponry falls . . . he wants to be very careful in that regard, and I happen to agree with him."