Options to reenter US from Toronto?

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Metrolinx has rail service between Niagara Falls, ON and Toronto several times a day, in answer to the question you posed.

Unlike your title, your actual question did not address crossing the border but was about a trip wholly inside of Canada. The Maple Leaf currently originates and terminates at Niagara Falls, NY, and does not cross into Canada at all.

To cross the border, I'd take a taxi between the Metrolinx/VIA station and the Rainbow Bridge and walk across. If you are taking the Maple Leaf or other Empire Service train take another taxi to the Niagara Falls, NY Amtrak station.
 
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You don't clear customs as part of your rail journey. No trains cross the border at present. No pedestrian traffic is allowed on the adjacent Whirlpool Bridge which is used by the Maple Leaf in better times, it is only open to NEXUS members in cars. You have to get from the station to the Rainbow Bridge, clear customs as a pedestrian, then get to the Amtrak station (if going from Canada to the US).
 
The one advantage of crossing as a pedestrian or by car is that, unlike arriving by air, the US does not require COVID testing to enter at land crossings.

Note that Canada has uniform requirements for all modes and requires a negative PCR test within 72 hours. For land crossing that means within 72 hours of presenting yourself at the primary inspection booth.

And don't forgot to complete the ArriveCan app in advance. If you haven't done the ArriveCan before arriving, you will not be eligible for the vaccine exemption from the 14 day quarantine requirement even if you are vaccinated.
 
Is the Maple Leaf running out of Niagara Falls? If so, does anyone know how to get to Niagara Falls, Ontario from Toronto?
It partly depends on the day of the week. GO runs four trains on Saturdays and Sundays from Union Station in Toronto to Niagara Falls ON. On weekdays you can get the train only as far as (I think) Burlington or Hamilton, with a connecting bus onwards. You then have to get yourself over to Niagara Falls NY - as Zephyr17 suggests.
 
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