After discussions with Lebanese Prime Minister Tammam Salam during a visit to Beirut, Müller announced that €55 million would be available immediately to aid large number of refugees in Lebanon.
There are currently more than 1.2 million Syrian refugees in Lebanon - a country of just 5.4 million - and Müller was shocked by the extent of the humanitarian crisis.
"This beats anything I have ever seen before" he said while in Beirut on Thursday.
The money will be used to fund the water supplies, food provisions and schools.
In addition Germany will offer a further €52m at the upcoming donors' conference for Syrian refugees in Kuwait, which will go towards aiding those displaced across the region.
During talks with local representatives, Müller heard about the burden on local infrastructure caused by the crisis.
Some of the money will therefore go towards locals in areas particularly affected by the mass displacement.
Because of the vast numbers of Syrian refugees who have fled to Lebanon, the Lebanese government effectively closed the borders in January in order to prevent Lebanon from buckling under the pressure.
Since 2012 Germany has contributed €250 million for humanitarian projects in Lebanon.
But the scale of the humanitarian aid required is even higher.
In a report published by Save The Children, the estimates of the cost of just replacing damaged, destroyed and occupied schools in Syria were almost €3 billion.
Earlier on in his visit Müller also went to a Palestinian refugee camp in Beirut, where Syrians have also been taken in.
On Friday Müller will visit a camp in Turkey.