No, that will not get it accurate enough, but depends on what you are wanting to do. If you are just looking to find the beginning of the compression stroke that will work. However, it is very difficult (really not possible) to get the location within several degrees of where you want to be. If your crank pulley is already marked and you know what the mark is and you trust it, this would be OK. If you want to mark a true TDC you need to use a procedure something like the following to find it.
You will need a pointer attached to the block with a sturdy point near the pulley. You then need some type of hard stop in the cylinder to stop the number 1 piston against. This can be a little bit of a challenge with a flathead. Need to be carful to not damage anything, I would use something like a bent brass rod through a spark plug hole. You need to be sure it remains in the same relative area during checking. Turn the engine one direction until it comes up against the stop and mark the crank pulley under the pointer. Then turn the engine in the opposite direction until it again comes up against the stop and mark that spot. TDC will be half way between the two marks. That location needs to be permanently marked on the pulley (file a notch in the pulley). Because the engine passes TDC twice per four cycles, the valve positions are not relevant when finding this location on the pulley (it does matter when you are setting the timing). It would be a good idea to check it several times to be sure you are getting repeatable results.
This will give you a marker for TDC and would require a dial back timing light to determine the engine timing. Another approach is to measure the diameter of the pulley and determine it's circumference. Divide the circumference by 360 and that is the distance around the outside edge of the pulley for 1 degree. You can then mark it in degrees out to say 25-30 degrees or every 2 degrees or 5 degrees or just a couple of convent locations, what every works for you.