Foreign Affairs Minister John Baird calls the aid "unprecedented" and says it is aimed at helping Jordan take care of the thousands of Syrian refugees streaming across its borders while dealing with its own economic challenges.
The support consists of $75 million over three years to help Jordan promote job creation and economic development.
Another $25 million is to help Jordan beef up security at sprawling refugee camps and protect Jordanians against potential chemical and biological weapons attack by the Syrian government.
This is latest — and largest —infusion of aid to Jordan since the Syrian civil war started two years ago.
Canada has previously committed just over $16 million to help Jordan cope with the fallout.
"The challenges facing Jordan are monumental in scope," Baird said in a written statement.
"Compassion for Syrians fleeing the death and destruction ravaging their homeland cannot be Jordan's undoing."
The G8 leaders' summit in Northern Ireland is expected to discuss a co-ordinated response to the Syrian crisis.
The United States is reportedly considering imposing a no-fly zone over Jordan while France and others are suggesting a NATO military response may be necessary.
In an interview with CTV's Question Period, Baird side-stepped whether Canada would participate in such measures. Rather, he stressed Canada's focus on providing humanitarian aid.
"This is the worst humanitarian tragedy of the 21st Century and obviously Canada wants to be there to do our part to support the victims of (Syrian President Bashar) Assad's brutality," he said.