As long as you have confirmed that the TDC mark on the pulley is accurate, then I see no reason not to use it to set your timing belt. However, the right way to do it would involve removing the front cover, which I believe requires you to take off the pully, which is only four small bolts anyway. Keep in mind that if the engine you are working on has a balance shaft or a shaft that drives a distributor, you'll want all that open so you can see in there anyway.
I usually set all the pistons halfway down the bore, and TDC the crank when the head is back on, and you are ready to put your belt back on. That will prevent any piston to valve contact while doing the work.
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